Ethylene-based polymer, polyethylene-based resin composition and use thereof, catalyst component for olefin polymerization, olefin polymerization catalyst containing the component, and method for producing ethylene-based polymer by using the catalyst

[0001] This application is a 371 of PCT/JP2012/058491, filed Mar. 29, 2012, the disclosure of which is incorporated herein by reference in its entirety. This application claims priority to Japan Patent Application 2011-073937, filed Mar. 30, 2011; and Japan Patent Application 2011-073945, filed Mar. 30, 2011, the disclosure of which are incorporated herein by reference in their entireties.

[0002] The present invention relates to an ethylene-based polymer having a developed long-chain branched structure and excellent in the moldability. As another aspect of the present invention, the present invention relates to a novel polyethylene-based resin composition and use thereof. More specifically, the present invention relates to a polyethylene-based resin composition excellent in the moldability and capable of producing a molded product excellent in the balance between impact strength and stiffness as well as in the transparency, and a molded product and a film each obtained by the injection molding, compression-injection molding, rotational molding, extrusion molding, hollow molding or blow molding of the polyethylene-based resin composition. Furthermore, the present invention relates to an olefin polymerization catalyst component containing a specific metallocene compound, an olefin polymerization catalyst containing the component, and a method for producing an olefin-based polymer by using the catalyst.

[0003] Recently, a film, a sheet, an injection molded product, a pipe, an ejection molded product, a hollow molded product and the like, which are made of a plastic, are used actively in various industrial fields. Among others, a polyethylene-based resin (ethylene-based polymer) finds widespread use, because this is, for example, inexpensive, lightweight and excellent in the moldability, stiffness, impact strength, transparency, chemical resistance and recyclability. In general, molding of the polyethylene-based resin is preformed in a molten state. However, in the case of an ethylene-based polymer alone, its melting characteristics may be insufficient, for example, in terms of flowability or the elongational viscosity may be inadequate, and in many cases, sufficient moldability can be hardly ensured or solid physical properties such as transparency and stiffness may lack.

[0004] As for the measure taken to compensate these deficiencies, a high-pressure polyethylene (HPLD) excellent in the moldability or an ethylene-based polymer differing in the molecular weight or density has been blended to improve the melting characteristics or solid physical properties (see, for example, Patent Documents 1 to 3).

[0005] Such a blend (ethylene-based resin composition) may satisfy the moldability but has a problem that reduction in the impact strength may be caused due to blending of HPLD or the molecular weight distribution or copolymerization composition distribution may be broadened to worsen the transparency.

[0006] Also, due to enforcement of the Containers Recycle Law or recent trend of resource saving, the amount of a raw material resin used needs to be reduced and from this standpoint, the demand for reduction in the wall thickness of a molded product is increasing, but in order to reduce the wall thickness, the stiffness (modulus) as well as the impact strength must be improved.

[0007] As the method for improving the impact strength, a method of reducing the density of the ethylene-based polymer is well known, but this method is disadvantageous in that the stiffness is also reduced (the polymer becomes soft), and for the purpose of reducing the wall thickness, there has been made, for example, an attempt to use a three-component blend composition obtained by further adding a specific HPLD to a combination of two kinds of specific ethylene·α-olefin copolymers differing in the density so as to enhance the moldability or transparency (see, for example, Patent Document 4).

[0008] According to this method, a polyethylene resin composition more excellent in the balance between impact strength and stiffness and also in the transparency than conventional compositions may be obtained, but the impact strength is unavoidably reduced due to blending of HPLD and furthermore, from the standpoint of stably supplying a product of constant quality in industrial level, a blend of three kinds of ethylene-based polymers is considered to be economically disadvantageous as compared with conventional compositions.

[0009] On the other hand, as to the method for improving the moldability, an attempt to introduce a long-chain branched structure capable of increasing the melt viscosity into an ethylene-based polymer has been made, but since the design for optimizing the long-chain branched structure is insufficient, reduction in the strength or transparency still cannot be avoided and the improvement level of moldability is yet low (see, for example, Patent Documents 5 to 8).

[0010] The polyolefin produced using a metallocene catalyst for olefin polymerization has a high uniformity in the polymer molecular structure such as molecular weight distribution or copolymerization composition distribution and is excellent in various mechanical properties such as impact strength and long lifetime and therefore, the amount used thereof is recently increasing. The metallocene-based polyolefin is excellent in various mechanical properties but, because of its narrow molecular weight distribution, is poor in the characteristics important to molding of a polyolefin, such as melt tension and melt flowability, and cannot satisfy sufficient performance in terms of mold processing.

[0011] As the method for improving the insufficient mold processability of the metallocene-based polyolefin, a method where the melt viscosity is increased by introducing a long-chain branch into a polyethylene by a polymerization reaction using a specific metallocene complex and the flowability or melt tension is thereby improved, is well known (see, for example, Patent Document 9). With respect to the specific metallocene complex for introducing a long-chain branch, a method using a bridged bisindenyl complex (see, for example, Patent Documents 10 to 13) or a constrained geometry half-metallocene complex (see, for example, Patent Document 14) is well known, but the long-chain branch obtained by such a method does not develop as in the structure of HPLD, and the improvement of melt viscosity of the polymer is not sufficient.

[0012] Also, as to the method for introducing a long-chain branch by a metallocene complex other than those described above, a method for producing a long-chain branch-containing polyethylene by using a bridged metallocene catalyst having a specific structure is known (see, for example, Patent Document 15), and specifically, an example of simultaneously using two kinds of metallocene complexes of dimethylsilylbis(pentadienyl)zirconium dichloride and diphenylmethylene(cyclopentadienyl)(fluorenyl)zirconium dichloride is shown. As the improved technology thereof, furthermore, a catalyst where the above-described two kinds of complexes are co-supported on the same support (see, for example, Patent Documents 16 to 18), and a catalyst where the kind of the complex combined is improved (see, for example, Patent Documents 19 and 20), are known. In these methods, it is supposed that one kind of a complex produces a polymer having a polymerizable double bond at the terminal (so-called macromer) and another complex is a complex excellent in the copolymerizability and copolymerizes with the macromer to form a long-chain branched structure.

[0013] Such a method may achieve introduction of a branched structure that is somewhat more developed than the long-chain branched structure by the conventional metallocene complex, but the level of development is still insufficient or those two kinds of metallocene complexes greatly differ in the copolymerizability of a comonomer, giving rise to a problem that the copolymerization composition distribution of the produced polymer may be broadened or the mechanical properties may deteriorate in association with production of a low-melting-point polymer.

[0014] Patent Document 21 has reported that when homopolymerization of ethylene is performed according to solution polymerization by using an asymmetric metallocene in which a cyclopentadienyl group and an indenyl group are carbon-bridged and methylaluminoxane, a branch-containing polyethylene can be produced, but the carbon number indicative of the branch length is from 1 to 20. Thus, the branch length is too short to exert an effect of improving mold processability as a long-chain branch, failing in exhibiting strain hardening of the elongational viscosity.

[0015] Also, Patent Document 22 has reported polymerization of propylene by a polymerization catalyst prepared by combining an asymmetric metallocene compound in which a cyclopentadienyl group and an indenyl group, each having a specific substituent, are bridged, with methylaminoxane, but this document is silent on the possibility of producing a long-chain branch when the polymerization above is applied to polymerization of ethylene, and the effect of improving the mold processability cannot be expected.

[0016] Furthermore, Patent Document 23 has reported a catalyst system capable of producing an ethylene polymer and an ethylene/butene copolymer, which are useful as a macromonomer, by using, out of asymmetric metallocenes in which a cyclopentadienyl group and an indenyl group are silicon-bridged, a metallocene having a methyl group on the 2-, 4- and 7-positions of the indenyl group and a modified clay compound, but the number of terminal double bonds of the polymer is small, and this document is silent on the possibility of producing a long-chain branch by this catalyst alone.

[0017] Recently, the present inventors have reported in Patent Document 24a method for producing an ethylene-based polymer improved in the mold processability by using a supported catalyst for olefin polymerization comprising, as an essential component, out of asymmetric metallocenes in which a cyclopentadienyl group and an indenyl group are bridged by a bridging group, a specific asymmetric metallocene having no substituent except for the bridging group on the cyclopentadienyl group and having a hydrogen atom or a specific substituent on the 3-position of the indenyl group. According to this method, an ethylene-based polymer having a large degree of strain hardening of the elongational viscosity is obtained and therefore, the mold processability is improved as compared with the conventional long-chain branched polyethylene, but since the long-chain branching index does not reach that of a high-pressure low-density polyethylene, more improvement of the long-chain branched structure is demanded.

[0018] Under these circumstances, it is required to solve the problems of the conventional ethylene-based resin composition and develop a polyethylene-based resin composition excellent in the moldability and capable of producing a molded product excellent in the balance between impact strength and stiffness as well as in the transparency. Furthermore, in order to solve the problems of a long-chain branch-containing polyethylene in conventional techniques and improve the mold processability of a metallocene-based polyethylene, it is required to develop an ethylene-based polymer having introduced thereinto a sufficiently large number of appropriate-length long-chain branches, an olefin polymerization catalyst excellent in the introduction of long-chain branch, and a production method of an olefin-based polymer.

[0019] Patent Document 1: JP-A-7-149962 (the term “JP-A” as used herein means an “unexamined published Japanese patent application”)

[0020] Patent Document 2: JP-A-9-31260

[0021] Patent Document 3: JP-A-2006-312753

[0022] Patent Document 4: JP-A-2010-31270

[0023] Patent Document 5: International Publication No. 97/10295

[0024] Patent Document 6: JP-A-2006-63325

[0025] Patent Document 7: JP-A-2006-124567

[0026] Patent Document 8: JP-A-2007-197722

[0027] Patent Document 9: JP-A-2-276807

[0028] Patent Document 10: JP-A-8-48711

[0029] Patent Document 11: JP-A-8-311260

[0030] Patent Document 12: JP-A-2004-149760

[0031] Patent Document 13: JP-A-2004-217924

[0032] Patent Document 14: JP-A-6-306121

[0033] Patent Document 15: JP-A-7-252311

[0034] Patent Document 16: JP-A-2006-233208

[0035] Patent Document 17: JP-A-2006-321991

[0036] Patent Document 18: JP-T-2007-520597 (the term “JP-T” as used herein means a published Japanese translation of a PCT patent application)

[0037] Patent Document 19: JP-T-2002-515521

[0038] Patent Document 20: JP-A-2009-144148

[0039] Patent Document 21: JP-A-5-043619

[0040] Patent Document 22: JP-A-7-224079

[0041] Patent Document 23: JP-A-2008-050278

[0042] Patent Document 24: JP-A-2011-137146

[0043] An object of the present invention is, considering the above-described problems of conventional techniques, to provide an ethylene-based polymer improved in the mold processability. Another object of the present invention is, considering the above-described problems of conventional techniques, to provide a polyethylene-based resin composition excellent in the molding characteristics and at the same time, excellent in the balance between impact strength and stiffness as well as in the transparency; provide a molded product excellent in the balance between impact strength and stiffness and also in the transparency, which is obtained by the injection molding, compression-injection molding, rotational molding, extrusion molding, hollow molding, blow molding or inflation molding of the polyethylene-based resin composition; and provide use of the molded product. Still another object of the present invention is to provide an olefin polymerization catalyst component capable of producing a metallocene-based polyolefin or a metallocene-based polyethylene, in which a sufficiently large number of appropriate length long-chain branches are introduced so as to improve the mold processability of a metallocene-based polyolefin, particularly a metallocene-based polyethylene; an olefin polymerization catalyst containing the component; and a method for producing an olefin-based polymer by using the catalyst.

[0044] Incidentally, in the present invention, the polyethylene is a general term of an ethylene homopolymer and a copolymer of ethylene and the later-described olefin and can be restated as an ethylene-based polymer.

[0045] As a result of a number of intensive studies to attain the above-described objects, the present inventors have found that when a specific ethylene-based polymer having a small amount of long-chain branched structure characterized by the elongational viscosity behavior and a specific ethylene-based polymer having a specific long-chain branched structure similarly characterized by the elongational viscosity behavior are combined and these two polymers are blended to give a specific MFR and a specific density, the obtained polyethylene-based resin composition exhibits good characteristics capable of solving the above-described problems. The present inventors have been accomplished based on this finding.

[0046] That is, according to a first aspect of the present invention, an ethylene-based polymer satisfying the following condition (B-1′) to condition (B-6) is provided.

[0047] (B-1′) MFR_B=0.001 to 200 g/10 min,

[0048] (B-2″) Density_B=0.880 to 0.970 g/cm³,

[0049] (B-3) [Mw/Mn]_B=2.0 to 10.0,

[0050] (B-4′) in a double logarithmic plot of elongational viscosity η(t) (unit: Pa·sec) and elongation time t (unit: sec) measured at a temperature of 170° C. and an elongational strain rate of 2 (unit: 1/sec), an inflection point of the elongational viscosity attributable to strain hardening is not observed, or when the inflection point is observed, assuming that the maximum elongational viscosity after strain hardening is η_B;Max(t₁) and the approximate straight line of the elongational viscosity before hardening is η_B;Linear(t), the degree of strain hardening [λmax(2.0)]_B defined by η_B;Max(t₁)/η_B;Linear(t₁) is from 1.2 to 30.0,

[0051] (B-5) the ratio [λmax(2.0)]_B/[λmax(0.1)]_B of [λmax(2.0)]_B defined in the same manner as in the condition (B-4′) and [λmax(0.1)]_B measured similarly by setting the elongational strain rate to 0.1 (unit: 1/sec) is from 1.2 to 10.0, and

[0052] (B-6) the polymer is produced by an ethylene polymerization reaction using a transition metal-containing catalyst.

[0053] According to a second aspect of the present invention, the ethylene-based polymer in the first aspect of the present invention, further satisfying at least one of the following condition (B-7) and condition (B-8) is provided:

[0054] (B-7) the branching index (g_C′) at a molecular weight of 1,000,000 as measured by a GPC measurement apparatus combining a differential refractometer, a viscosity detector and a light scattering detector is from 0.30 to 0.70, and

[0055] (B-8) the content (W_C) of components having a molecular weight of 1,000,000 or more as measured by a GPC measurement apparatus combining a differential refractometer, a viscosity detector and a light scattering detector is from 0.01 to 30%.

[0056] According to a third aspect of the present invention, a polyethylene-based resin composition comprising: (A) from 41 to 99 wt % of an ethylene-based polymer satisfying the following condition (A-1) to condition (A-4); and (B) from 1 to 59 wt % of the ethylene-based polymer claimed in claim 1 or 2, wherein MFR of the composition as a whole is from 0.05 to 50 g/10 min and the density is from 0.910 to 0.960 g/cm³, is provided:

[0057] (A-1) MFR_A=0.3 to 100 g/10 min,

[0058] (A-2) Density_A=0.915 to 0.970 g/cm³,

[0059] (A-3) [Mw/Mn]_A=2.0 to 10.0, and

[0060] (A-4) in a double logarithmic plot of elongational viscosity η(t) (unit: Pa·sec) and elongation time t (unit: sec) measured at a temperature of 170° C. and an elongational strain rate of 2 (unit: 1/sec), an inflection point of the elongational viscosity attributable to strain hardening is not observed, or when the inflection point is observed, assuming that the maximum elongational viscosity after strain hardening is η_A;Max(t₁) and the approximate straight line of the elongational viscosity before hardening is η_A;Linear(t), the degree of strain hardening [λmax(2.0)]_A defined by η_A;Max(t₁)/η_A;Linear(t₁) is from 1.0 to 2.0.

[0061] According to a fourth aspect of the present invention, the polyethylene-based resin composition in the third aspect of the present invention, wherein said ethylene-based polymer (B) satisfies the following condition (B-1) to condition (B-6), is provided:

[0062] (B-1) MFR_B=0.01 to 1.5 g/10 min and 100>MFR_A/MFR_B>1.0,

[0063] (B-2) Density_B=0.880 to 0.940 g/cm³,

[0064] (B-3) [Mw/Mn]_B=2.0 to 10.0,

[0065] (B-4) [λmax(2.0)]_B defined in the same manner as in the condition (A-4) of the third aspect of the present invention is from 1.2 to 20.0 and 20>[λmax(2.0)]_B/[λmax(2.0)]_A>1.0,

[0066] (B-5) the ratio [λmax(2.0)]_B/[λmax(0.1)]_B of [λmax(2.0)]_B defined in the same manner as in the condition (A-4) of the third aspect of the present invention and [λmax(0.1)]_B measured similarly by setting the elongational strain rate to 0.1 (unit: 1/sec) is from 1.2 to 10.0, and

[0067] (B-6) the polymer is produced by an ethylene polymerization reaction using a transition metal-containing catalyst.

[0068] According to a fifth aspect of the present invention, the polyethylene-based resin composition in the third aspect of the present invention, wherein said ethylene-based polymer (B) further satisfies the following condition (B-2′), is provided:

[0069] (B-2′) 1.070>density_A/density_B>0.990.

[0070] According to a sixth aspect of the present invention, the polyethylene-based resin composition in the third aspect of the present invention, wherein said ethylene-based polymer (A) is an ethylene polymer or ethylene.α-olefin copolymer produced by homopolymerization of ethylene or copolymerization with an α-olefin caused by a Ziegler-Natta catalyst produced using a magnesium compound and a titanium compound, is provided.

[0071] According to a seventh aspect of the present invention, a molded product obtained by an injection molding, compression-injection molding, rotational molding, extrusion molding, hollow molding or blow molding of the polyethylene-based resin composition in the third aspect of the present invention, is provided.

[0072] According to an eighth aspect of the present invention, a film obtained by an extrusion molding, hollow molding, blow molding or inflation molding of the polyethylene-based resin composition in the third aspect of the present invention.

[0073] According to a nineth aspect of the present invention, an olefin polymerization catalyst component comprising the following component (A-1b) and component (A-2b), is provided:

[0074] Component (A-1b): a metallocene compound represented by the following formula (1b):

[0075]
[in formula (1b), M^1b represents any one transition metal of Ti, Zr and Hf; each of X^1b and X^2b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; each of Q^1b and Q^2b independently represents a carbon atom, a silicon atom or a germanium atom; each R^1b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and at least two members out of four R^1b may combine to form a ring together with Q^1b and Q^2b; m^b is 0 or 1 and when m^b is 0, Q^1b is bonded directly to the conjugated 5-membered ring including R^2b and R^3b; and each of R^2b, R^3b and R^4b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40 and out of R^2b, R^3b and R^4b, only either one pair of adjacent R^3b and R^3b and adjacent R^2b and R^3b may form a ring together with the carbon atoms to which the pair is bonded], and

[0076] Component (A-2b): a metallocene compound represented by the following formula (2b):

[0077]
[in formula (2b), M^2b represents any one transition metal of Ti, Zr and Hf; each of X^11b and X^12b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; Q^11b represents a carbon atom, a silicon atom or a germanium atom; each R^11b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and two R^11b may combine with each other to form a ring together with Q^11b; each of R^12b, R^14b and R^15b independently represents an atom or a group selected from a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, and a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, provided that at least one member is not a hydrogen atom; each R^13b independently represents a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40; and out of R^12b, R^13b, R^14b and R^15b, any only one pair of adjacent R^12b and R^12b, adjacent R^13b and R^13b and adjacent R^12b and R^13b and any only one pair of adjacent R^14b and R^14b, adjacent R^15b and R^15b and adjacent R^14b and R^15b may form a ring together with the carbon atoms to which the pair is bonded].

[0078] According to a tenth aspect of the present invention, an olefin polymerization catalyst component comprising a metallocene compound represented by the following formula (1c), is provided:

[0079]
[in formula (1c), M^1c represents any one transition metal of Ti, Zr and Hf; each of X^1c and X^2c independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; each of Q^1c and Q^2c independently represents a carbon atom, a silicon atom or a germanium atom; each R^1c independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and at least two members out of four R^1c may combine to form a ring together with Q^1c and Q^2c; m^c is 0 or 1 and when m^c is 0, Q^1c is bonded directly to the conjugated 5-membered ring including R^2c; each of R^2c and R^4c independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20; and R^3c represents a substituted aryl group represented by the following formula (1-ac)]:

[0080]
[in formula (1-ac), Y^1c represents an atom of Group 14, Group 15 or Group 16 of the periodic table; each of R^5c, R^6c, R^7c, R^8c and R^9c independently represents a hydrogen atom, a fluorine atom, a chlorine atom, a bromine atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing oxygen or nitrogen and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, an alkoxy group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20; adjacent groups of R^5c, R^6c, R^7c, R^8c and R^9c may combine with each other to form a ring together with the atoms bonded to these groups; n^c is 0 or 1 and when n^c is 0, the substituent R^5c is not present on Y^1c; and p^c is 0 or 1 and when p^c is 0, the carbon atom to which R^7c is bonded and the carbon atom to which R^9c is bonded are bonded directly; provided that when Y^1c is a carbon atom, at least one of R^5c, R^6c, R^7c, R^8c and R^9c is not a hydrogen atom].

[0081] According to an eleventh aspect of the present invention, an olefin polymerization catalyst comprising the olefin polymerization catalyst component in the nineth or tenth aspect of the present invention, is provided.

[0082] According to a twelfth aspect of the present invention, a production method of an ethylene-based polymer, comprising producing an ethylene-based polymer satisfying at least the condition (B-4′) among the conditions in the first aspect of the present invention by using an olefin polymerization catalyst containing the following components (A) and (B), is provided:

[0083] Component (A): at least any one of the following catalyst components (A-i) to (A-iii):

[0084] (A-i) the olefin polymerization catalyst component in the nineth aspect of the present invention,

[0085] (A-ii) the olefin polymerization catalyst component in the tenth aspect of the present invention, and

[0086] (A-iii) an olefin polymerization catalyst component containing a metallocene compound represented by the following formula (1d):

[0087]
[in formula (1d), M^1d represents any one transition metal of Ti, Zr and Hf; each of X^1d and X^2d independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; each of Q^1d and Q^2d independently represents a carbon atom, a silicon atom or a germanium atom; each R^1d independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and at least two members out of four R^1d may combine to form a ring together with Q^1d and Q^2d; m^d is 0 or 1 and when m^d is 0, Q^1d is bonded directly to the conjugated 5-membered ring including R^2d and R^3d; each of R^2d and R^3d represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20, provided that at least one R^2d is not a hydrogen atom; R^4d represents a saturated or unsaturated divalent hydrocarbon group having a carbon number of 4 or 5 for forming a condensed ring with the 5-membered ring to which R^4d is bonded; R^5d is an atom or a group bonded to a carbon atom of R^4d and each independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20; and n^d represents an integer of 0 to 10 and when n^d is 2 or more, at least two R^5d may form a ring together with the carbon atoms to which R^5d are bonded], and

[0088] Component (B): a compound capable of reacting with a metallocene compound of the component (A) to produce a cationic metallocene compound.

[0089] According to a thirteenth aspect of the present invention, the ethylene-based polymer in the first aspect of the present invention, which is produced by the production method of an ethylene-based polymer in the twelfth aspect of the present invention, is provided.

[0090] According to a fourteenth aspect of the present invention, the polyethylene-based resin composition in the third aspect of the present invention, wherein said ethylene-based polymer is the ethylene-based polymer in the thirteenth aspect of the present invention, is provided.

[0091] According to the present invention, an ethylene-based polymer having a developed long-chain branched structure and excellent in the moldability can be provided.

[0092] The polyethylene-based resin composition of the present invention has excellent molding characteristics and at the same time, has an effect that the balance between impact strength and stiffness is excellent and furthermore, the transparency is excellent. In addition, the molded product by the injection molding, compression-injection molding, rotational molding, extrusion molding, hollow molding, blow molding or inflation molding of the polyethylene-based resin composition is also excellent in the balance between impact strength and stiffness as well as in the transparency, so that a molded product reduced in the wall thickness can be provided in an industrially advantageous manner.

[0093] Moreover, according to the present invention, a method for producing a metallocene-based polyolefin or metallocene-based polyethylene having a sufficiently large number of appropriate-length long-chain branches, wherein an olefin polymerization catalyst component containing a specific metallocene compound is prepared and the catalyst component is used for an olefin polymerization catalyst, can be provided. In turn, a method for improving the mold processability of a metallocene-based polyethylene can be provided.

[0098] The present invention relates to a polyethylene-based resin composition obtained by blending a specific ethylene-based polymer (A) having a small amount of long-chain branched structure characterized by the elongational viscosity behavior and a specific ethylene-based polymer (B) having a specific long-chain branched structure similarly characterized by the elongational viscosity behavior to give a specific MFR and a specific density; a molded product obtained by molding the polyethylene-based resin composition; and use of the molded product. The present invention is described below item by item.

[I] Polyethylene-Based Resin Composition of the Present Invention

[0099] The polyethylene-based resin composition of the present invention is characterized by containing from 41 to 99 wt % of (A) an ethylene-based polymer satisfying specific conditions (A-1) to (A-4) (hereinafter, sometimes simply referred to as component (A)) and from 1 to 59 wt % of (B) an ethylene-based polymer satisfying specific conditions (B-1) to (B-6) (hereinafter, sometimes simply referred to as component (B)), wherein MFR of the composition as a whole is from 0.05 to 50 g/10 min and the density is from 0.910 to 0.960 g/cm³. Respective components constituting the polyethylene-based resin composition of the present invention, characteristics thereof, and the like are described below.

[0100] The compound (A) that is one of components constituting the polyethylene-based resin composition of the present invention satisfies all of the conditions (A-1) to (A-4) described below.

1-1. Condition (A-1)

[0101] The melt flow rate (MFR_A) of the component (A) in the present invention is from 0.3 to 100 g/10 min, preferably from 0.9 to 20 g/10 min, more preferably from 1.4 to 10 g/10 min.

[0102] If MFR_A is less than 0.3 g/10 min, the polyethylene-based resin composition may be inferior in the moldability, particularly in the melt flowability and spreadability, and if MFR_A exceeds 100 g/10 min, the polyethylene-based resin composition or its molded product may be disadvantageously reduced in the mechanical strength such as impact strength, tear strength and tensile strength. Incidentally, in the present invention, MFR of the ethylene-based polymer and polyethylene-based resin composition indicates a value when measured under the conditions of 190° C. and a load of 21.18 N (2.16 kg) in accordance with “Test Method for Melt Flow Rate (MFR) and Melt Volume Flow Rate (MVR) of Plastics-Thermoplastics” of JIS K7210.

1-2. Condition (A-2)

[0103] The density_A of the ethylene-based polymer (A) in the present invention is from 0.915 to 0.970 g/cm³, preferably from 0.917 to 0.950 g/cm³, more preferably from 0.925 to 0.940 g/cm³.

[0104] When the density_A is in this range, the polyethylene-based resin composition or its molded product is excellent in the balance between impact strength and stiffness and in the transparency. On the other hand, if the density_A is less than 0.915 g/cm³, the stiffness is reduced and when the product is a molded product having a small thickness, such as film and sheet, as well as various problems in using the product, a problem is disadvantageously brought about in the step of winding up the product or the post-processing step such as surface printing•lamination or when the product is a molded product having a large wall thickness, such as pipe and various containers, since the product is too soft and undergoes deformation, the wall thickness must be disadvantageously designed to be larger than necessary. Also, if the density_A exceeds 0.970 g/cm³, the impact strength or transparency is deteriorated and this is not preferred. Incidentally, in the present invention, the density of the ethylene-based polymer or the polyethylene-based resin composition indicates a value when measured by the following method.

[0105] Pellets are hot-pressed to prepare a 2 mm-thick press sheet, and this sheet is placed in a beaker having a volume of 1,000 ml. The beaker is filled with distilled water, covered with a watch glass, heated by a mantle heater and after coming to a boil, the distilled water was boiled for 60 minutes. Thereafter, the beaker is placed on a wooden table and allowed to cool. In this operation, the amount of the boiling distilled water after boiling for 60 minutes is set to 500 ml, and the period of time until reaching room temperature is adjusted not to fall below 60 minutes. Furthermore, the test sheet is immersed in a nearly central part of the water while keeping it away from contact with the beaker or water surface. The sheet is annealed for 16 to 24 hours under the conditions of 23° C. and a humidity of 50%, then punched into 2-mm squares, and measured at a test temperature of 23° C. in accordance with “Test Method for Density and Specific Gravity of Plastics-Unfoamable Plastics” of JIS K7112.

1-3. Condition (A-3)

[0106] The ratio ([Mw/Mn]_A) between weight average molecular weight (Mw) and number average molecular weight (Mn) of the component (A) in the present invention is from 2.0 to 10.0, preferably from 2.5 to 10.0, more preferably from 2.9 to 5.0. If [Mw/Mn]_A is less than 2.0, the polyethylene-based resin composition may be inferior in the moldability, particularly in the melt flowability, or the polymer may be difficult to mix with other polymer components and therefore, this should be avoided.

[0107] If [Mw/Mn]_A exceeds 10.0, the effect of improving the stiffness of the polyethylene-based resin composition or its molded product may be insufficient or the transparency may be deteriorated, and this is not preferred. Incidentally, in the present invention, each of Mw and Mn of the ethylene-based polymer or polyethylene-based resin composition indicates a value measured by gel permeation chromatography (GPC) method.

[0108] Conversion to molecular weight from retention volume is performed using a calibration curve prepared in advance with standard polystyrene. All of standard polystyrenes used are the following brands of Tosoh Corporation: F380, F288, F128, F80, F40, F20, F10, F4, F1, A5000, A2500 and A1000.

[0109] The calibration curve is prepared by injecting 0.2 mL of a solution after dissolving each standard polystyrene in ODCB (containing 0.5 mg/mL of BHT) to have a concentration of 0.5 mg/mL. As the calibration curve, a cubic expression obtained by approximation by the least square method is employed. For the viscosity expression ([η]=K×M^α) used in the conversion to the molecular weight, the following numerical values are used.

[0110] PS: K=1.38×10⁻⁴, α=0.7

[0111] PE: K=3.92×10⁻⁴, α=0.733

[0112] PP: K=1.03×10⁻⁴, α=0.78

[0113] Incidentally, the measurement conditions of GPC are as follows.

[0114] Instrument: GPC (ALC/GPC, 150C) manufactured by Waters

[0115] Detector: IR detector (measurement wavelength: 3.42 μm), MIRAN 1A, manufactured by FOXBORO

[0116] Column: AD806M/S (three) manufactured by Showa Denko

[0117] Moving phase solvent: o-dichlorobenzene

[0118] Measurement temperature: 140° C.

[0119] Flow rate: 1.0 ml/min

[0120] Injection volume: 0.2 ml

[0121] Preparation of sample: A 1 mg/mL solution of the sample is prepared using ODCB (containing 0.5 mg/mL of BHT) and dissolved over about 1 hour at 140° C.

[0122] Incidentally, a base line and a section of the obtained chromatogram are determined, for example, as shown in FIG. 1.

1-4. Condition (A-4)

[0123] The component (A) in the present invention satisfies the condition that in a double logarithmic plot of elongational viscosity η(t) (unit: Pa·sec) and elongation time t (unit: sec) measured at a temperature of 170° C. and an elongational strain rate of 2 (unit: 1/sec), an inflection point of the elongational viscosity attributable to strain hardening is not observed or when the inflection point is observed, assuming that the maximum elongational viscosity after strain hardening is η_Max(t₁) and the approximate straight line of the elongational viscosity before hardening is η^Linear(t), the degree of strain hardening [λmax(2.0)]_A defined by η_Max(t₁)/η_Linear(t₁) is from 1.0 to 2.0, preferably from 1.0 to 1.5, more preferably from 1.0 to 1.2, and in a most preferred case, the inflection point is not observed or [λmax(2.0)]_A is from 1.0 to 1.1. Here, the approximate straight line of the elongational viscosity before hardening is a tangent line having a smallest gradient (here, however, the gradient is 0 or a positive value) among tangent lines of a curve of the double logarithmic graph in the range of t corresponding to a strain amount of 0.2 to 1.0.

[0124] If [λmax(2.0)]_A is less than 1.0, the ethylene-based polymer, polyethylene-based resin composition or its molded product may be in a non-uniform molten state or may have a thermally unstable structure, and this is not preferred. If [λmax(2.0)]_A exceeds 2.0, the melt tension and flowability during molding may be excellent, but the polyethylene-based resin composition or its molded product may be disadvantageously reduced in the impact strength or transparency.

[0125] In general, a polyethylene is processed into an industrial product by a shaping method involving a molten state, such film molding, blow molding and foam molding, and at this time, the elongational flow characteristics represented by the above-described elongational viscosity or degree of strain hardening greatly affect the ease of molding.

[0126] That is, a polyethylene having a narrow molecular weight distribution and having no long-chain branch exhibits bad moldability because of its low melt strength, whereas a polyethylene having an ultrahigh molecular weight component or a long-chain branch component has a property of undergoing strain hardening during melt elongation, that is, abruptly rising in the elongational viscosity on the high strain side, and a polyethylene exhibiting this property outstandingly is excellent in the moldability. A polyethylene resin having such elongational flow characteristics has an effect of, for example, preventing uneven wall thickness or blown rupture of a product in the film molding or blow molding, enabling high-speed molding, or making it possible to raise the percentage of closed pores at the foam molding and provides for merits such as increase of strength of a molded article, enhancement of design property, reduction in weight, improvement of molding cycle, and elevation of heat insulating property. However, on the other hand, if the elongational flow characteristics are too strong, there may arise a problem, for example, the impact strength of the molded product may be reduced due to strength anisotropy that is presumed to be attributable to molecular orientation during molding, or the transparency may be deteriorated due to reduction in the surface smoothness of a molded product, which is presumed to be attributable to a property of the melt elasticity being too high.

[0127] As a result of intensive studies on a polyethylene-based resin composition with an attempt to improve the molding process bound up with the elongational flow characteristics of a polyethylene and overcome the problem in mechanical properties of a molded product by designing the long-chain branched structure as a main factor governing the elongational viscosity characteristics, it has been found that, as described above, when an ethylene-based polymer (A) having a small amount of long-chain branched structure is used as a high MFR main component of the resin composition, that is, as a main component on the low molecular weight side, the polymer is excellent in contribution to enhancement of mechanical properties, particularly stiffness, and furthermore, excellent in prevention of deterioration of the transparency.

[0128] With respect to the measurement method for the degree of strain hardening, as long as the uniaxial elongational viscosity can be measured, the same value is obtained in principle by any method, and details of the measurement method and measurement apparatus are described, for example, in known literature, Polymer, 42 (2001), 8663.

[0129] The measurement method and measurement apparatus preferred for measurement of the ethylene-based polymer of the present invention include the followings.

Measurement Method:

[0130] Apparatus: Ares manufactured by Rheometorics

[0131] Fixture: Extentional Viscosity Fixture, manufactured by T.A. Instrument

[0132] Measurement temperature: 170° C.

[0133] Strain rate: 2/sec

[0134] Preparation of test piece: A sheet having a size of 18 mm×10 mm and a thickness of 0.7 mm is prepared by press molding.

Calculation Method:

[0135] The elongational viscosity at 170° C. and a strain rate of 2/sec is plotted in a double logarithmic graph where the abscissa is the time t (sec) and the ordinate is the elongational viscosity η(Pa·sec). On this double logarithmic graph, assuming that the maximum elongational viscosity until reaching a strain amount of 4.0 after strain hardening is η_Max(t₁) (t₁ is the time at which the maximum elongational viscosity is shown) and the approximate straight line of the elongational viscosity before hardening is η_Linear(t), a value calculated as η_Max(t)/η_Linear(t₁) is defined as the degree of strain hardening (λmax). Incidentally, occurrence or no occurrence of strain hardening is judged by whether an inflection point at which the elongational viscosity is changed from an upwardly projecting curve to a downwardly projecting curve with the elapse of time is present or absent.

[0136] FIGS. 2 and 3 are plot diagrams of typical elongational viscosity. FIG. 2 is a case where an inflection point of elongational viscosity is observed, and η_Max(t₁) and η_Linear(t) are shown in the figure. FIG. 3 is a case where an inflection point of elongational viscosity is not observed.

1-5. Composition of Ethylene-Based Polymer (A)

[0137] The component (A) in the present invention is an ethylene homopolymer or a copolymer of ethylene and an α-olefin having a carbon number of 3 to 20. Examples of the α-olefin as a copolymerization component used here include propylene, butene-1,3-methylbutene-1,3-methylpentene-1,4-methylpenetene-1, pentene-1, hexene-1, heptene-1, octene-1, decene-1, tetradecene-1, hexadecene-1, octadecene-1, and eicocene-1. Only one of these α-olefins may be used, or two or more thereof may be used in combination. Among these, an α-olefin having a carbon number of 3 to 10 is preferred, and specific examples thereof include propylene, butene-1,3-methylbutene-1,4-methylpentene-1, pentene-1, hexene-1, heptene-1, octene-1, and decene-1. An α-olefin having a carbon number of 4 to 8 is more preferred, and specific examples thereof include butene-1,3-methylbutene-1,4-methylpentene-1, pentene-1, hexene-1, heptene-1, and octene-1. Particularly preferred α-olefins are butene-1, hexene-1, and octene-1. Incidentally, in the later-described olefin polymerization catalyst, even in the case of homopolymerization of ethylene, an α-olefin such as 1-butene and 1-hexene due to an ethylene oligomerization reaction may occur as a by-product in the polymerization system, or a reaction called “Chain-walking reaction” where a short-chain branch such as methyl group and ethyl group is produced in the main chain of an olefin polymer by an isomerization reaction of a bond between an active center metal and a terminal carbon at the growth terminal of olefin polymerization, is known, and the short-chain branched structure produced by such a reaction in the ethylene homopolymer is sometimes confused with the short-chain branched structure produced by copolymerization of an α-olefin.

[0138] Accordingly, the ethylene homopolymer as used in the present invention indicates a polymer produced as a result of polymerization proceeded without externally supplying an α-olefin as a comonomer, and the ethylene.α-olefin copolymer indicates a polymer produced as a result of polymerization performed by externally supplying the α-olefin. The term “ethylene-based polymer” is used for collectively referring to the ethylene homopolymer and the ethylene.α-olefin copolymer (including the later-described case of using, as a comonomer, a monomer except for an α-olefin).

[0139] The ratio of ethylene and an α-olefin in the ethylene-based polymer is from about 80 to 100 wt % of ethylene and from about 0 to 20 wt % of an α-olefin, preferably from about 85 to 99.9 wt % of ethylene and from about 0.1 to 15 wt % of an α-olefin, more preferably from about 90 to 99.5 wt % of ethylene and from about 0.5 to 10 wt % of an α-olefin, still more preferably from about 90 to 99 wt % of ethylene and from about 1 to 10 wt % of an α-olefin. When the ethylene content is in this range, the polyethylene-based resin composition or its molded product can have good balance between stiffness and impact strength.

[0140] The copolymerization may be any of alternate copolymerization, random copolymerization and block copolymerization. Of course, it is possible to use a small amount of a comonomer other than ethylene and an α-olefin, and in this case, the comonomer includes a compound having a polymerizable double bond, for example, styrenes such as styrene, 4-methylstyrene and 4-dimethylaminostyrene, dienes such as 1,4-butadiene, 1,5-hexadiene, 1,4-hexadiene and 1,7-octadiene, cyclic compounds such as norbornene and cyclopentene, and oxygen-containing compounds such as hexenol, hexenoic acid and methyl octenoate. However, in the case of using dienes, it is indisputable that the comonomer must be used within a range causing no development of a long-chain branched structure, that is, within a range satisfying the condition (A-4).

1-6. Production Method of Ethylene-Based Polymer (A)

[0141] As the component (A) in the present invention, an ethylene-based polymer having the composition above and satisfying all of the conditions (A-1) to (A-4) is produced and used. The production is performed by a method of homopolymerizing ethylene or copolymerizing ethylene with the above-described α-olefin, by using an olefin polymerization catalyst.

[0142] As the olefin polymerization catalyst, various kinds of catalysts are known at present, and the catalyst is not limited as long as the ethylene-based polymer (A) can be prepared within the limitations of the configuration of catalyst components and the design of polymerization conditions or post-processing conditions, but as an example of the technique suitable for the production of the ethylene-based polymer (A) and satisfying the profitability at the industrial level, specific examples include transition metal-containing catalysts for olefin polymerization described in the following (i) to (iv).

[0143] Examples of the olefin polymerization catalyst suitable for the production of the ethylene-based polymer (A) include a Ziegler-Natta catalyst that is an olefin coordination polymerization catalyst composed of a combination of a transition metal compound and an alkyl compound or the like of a typical metal. Above all, a so-called Mg—Ti type Ziegler catalyst in which a solid catalyst component obtained by loading a titanium compound on a magnesium compound and an organoaluminum compound are combined (refer, for example, to “Shokubai Katsyou Daijiten (Practical Dictionary of Catalysts); issued by Kogyo Chosakai, 2004” and “Shutsugan Keitou Zu—Olefin Jugo Shokubai no Hensen—(Application Flow Chart—History of Olefin Polymerization Catalyst—); issued by Japan Institute of Invention and Innovation, 1995”) is preferred, because this catalyst is inexpensive, highly active and excellent in the suitability for polymerization process.

[0144] Among others, an Mg/Ti catalyst supported on an inactive support material described in JP-A-54-142192 and JP-A-54-148093 is preferred. More specifically, examples thereof include a catalyst obtained by a process where a porous silica previously treated with triethylaluminum is impregnated with a uniform mixed solution of a tetrahydrofuran solution of anhydrous MgCl₂ and TiCl₃ or TiCl₄ and then dried to a solid state, and a catalyst obtained by applying preliminary olefin polymerization to an Mg/Ti catalyst in the presence of an organoaluminum described in JP-A-63-117019, for example, a preliminarily polymerized catalyst obtained by a process where a mixed solution of TiCl₄ and methylhydrogenpolysiloxane is introduced into a solid component obtained by the reaction of MgCl₂, Ti(OnBu)₄ and methylhydrogenpolysiloxane and the obtained catalyst is subjected to preliminary ethylene polymerization in the presence of triethylaluminum. Other examples include an olefin polymerization catalyst in which a low-valent titanium atom-containing catalyst component obtained by the reaction of a magnesium•aluminum composite material and a quadrivalent titanium compound is combined with an organoaluminum compound, described in JP-A-60-195108; a solid-state catalyst obtained by adding dropwise ethylaluminum sesquichloride or the like to a uniform mixture of magnesium ethoxide, tri-n-butoxy monochloroethane and n-butanol, described in JP-A-56-61406 and the like; and an olefin polymerization solid catalyst containing magnesium, a halogen atom, titanium and an electron donor, described in JP-A-2001-139635 and the like.

[0145] As an example of the polymerization catalyst suitable for the production of the ethylene-based polymer (A), a metallocene catalyst that is an olefin polymerization catalyst composed of a metallocene-based transition metal compound and a promoter component (see, for example, “Metallocene Shokubai ni-yoru Jisedai Polymer Kogyoka Gijutsu (Next-Generation Polymer Engineering Technology by Metallocene Catalyst) (Volume One and Two); issued by Inter-Research, 1994”) is used, because this catalyst is relatively inexpensive, highly active and excellent in the suitability for polymerization process and furthermore, an ethylene-based polymer having a narrow molecular weight distribution and a narrow copolymerization composition distribution is obtained.

[0146] Among others, an olefin polymerization catalyst system containing a so-called metallocene complex and an alumoxane, described in JP-A-60-35007 and the like, and a catalyst system using a promoter component other than alumoxane, described in JP-A-8-34809, JP-A-8-127613, JP-A-11-193306, JP-T-2002-515522 and the like, are suitably used. As the metallocene complex, those where the center metal is Ti, Zr or Hf belonging to Group 4B of the periodic table exhibit high activity for ethylene polymerization and therefore, are suitably used. As for the ligand structure of such a center metal, various structures are known at present and being examined for the polymerization performance such as molecular weight of the produced polyethylene and α-olefin copolymerizability. As described above, the ethylene-based polymer (A) of the present invention preferably has no or a small amount of long-chain branched structure and for the production of an ethylene-based polymer having such a property, a so-called non-bridged complex where a ligand having a conjugated 5-membered ring structure is not bridged with another ligand by a bridging group, is preferred. According to the structure classification of metallocene compounds by the following formulae [1], [2], [3] and [4] described, for example, in JP-A-11-310612, compounds represented by formulae [1] and [3] are preferred, and a compound represented by formula [1] is more preferred. However, a higher concentration at the polymerization site of ethylene or α-olefin and a shorter polymerization reaction time are supposed to be disadvantageous for the production of a long-chain branched structure and therefore, the propriety of the metallocene compound is of course limited to a relative degree contingent on performing the polymerization under the same conditions. In addition, metallocene complexes described, for example, in JP-A-5-132518, JP-A-2000-154196 and JP-A-2004-161760 are also suitably used. Furthermore, a metallocene complex having a heteroatom-containing monocyclic or polycyclic heteroaromatic group as a substituent on a ligand of a conjugated 5-membered ring structure, described, for example, in JP-T-2002-535339 is also suitably used.

[0147]
[wherein each of A¹ to A⁴ represents a ligand having a conjugated 5-membered ring structure (A¹ to A⁴ may be the same or different in the same compound), Q¹ represents a bonding group for bridging two conjugated 5-membered ring ligands at arbitrary positions, each of Z¹ and Z² independently represents a ligand containing a nitrogen, oxygen, silicon, phosphorus or sulfur atom bonded to M, a hydrogen atom, a halogen atom or a hydrocarbon group, Q² represents a bonding group for bridging Z² and an arbitrary position of the conjugated 5-membered ring ligand, M represents a metal atom selected from Group 4 of the periodic table, and each of X and Y independently represents a hydrogen atom, a halogen atom, a hydrocarbon group, an alkoxy group, an amino group, a phosphorus-containing hydrocarbon group or a silicon-containing hydrocarbon group, which is bonded to M; their details are as defined in the patent publication above].

[0148] The Phillips catalyst is a chromium catalyst where a chromium compound is supported on an inorganic oxide support such as silica, silica-alumina and silica-titania and at least a part of chromium elements supported is converted into a hexavalent chromium element by performing activation in a non-reducing atmosphere (see, for example, M. P. McDaniel, Advances in Catalysis, Volume 33, page 47, 1985, Academic Press Inc.; M. P. McDaniel, Handbook of Heterogeneous Catalysis, page 2400, 1997, VCH; M. B. Welch et al., Handbook of Polyolefins: Synthesis and Properties, page 21, 1993, Marcel Dekker). The Phillips catalyst exhibits high activity for ethylene polymerization and therefore, is suitably used. However, since the ethylene-based polymer produced using a Phillips catalyst tends to contain a long-chain branched structure or have a broad molecular weight distribution, its use as the ethylene-based polymer (A) of the present invention requires special care to satisfy the condition (A-3) or (A-4).

[0149] As an example of the polymerization catalyst suitable for the production of the ethylene-based polymer (A), a post-metallocene catalyst that is an olefin polymerization catalyst using a homogeneous metal complex (non-metallocene complex) except for the above-described metallocene-based transition metal compound (see, for example, “Polyethylene Gijutsu Dokuhon (Polyethylene Technology Guidebook; issued by Kogyo Chosakai Publishing, 2001”, “Kin'itsu-kei Sen'i Kinzoku Shokubai ni-yoru Living Jugo (Living Polymerization by Homogeneous Transition Metal Catalyst); issued by IPC, 1999”, and “Shokubai Katsuyo Daijiten (Practical Dictionary of Catalysts); issued by Kogyo Chosakai, 2004”) is used, because this catalyst is relatively inexpensive and excellent in the activity and furthermore, an ethylene-based polymer having a narrow molecular weight distribution and a narrow copolymerization composition distribution is obtained.

[0150] Among others, suitably used are bisimide, iminoamide and bisamide compounds of a transition metal having a 4- to 8-membered ring chelate structure that is formed by bonding a ligand having at least two N atoms to a transition metal belonging to Groups 3 to 11 of the periodic table through those two N atoms and contains the transition metal, disclosed, for example, in JP-T-10-513489, JP-T-2002-521538, JP-T-2000-516295, JP-T-2000-514132, Macromolecules, 1996, page 5241, JACS, 1997, 119, page 3830, JACS, 1999, 121, page 5798, and Organometallics, 1998, page 3155; bis-hydrocarbyloxy and bis-hydrocarbylthio compounds of a transition metal having a 4- to 8-membered ring chelate structure that is formed by bonding a ligand having at least two O or S atoms to a transition metal belonging to Groups 3 to 11 of the periodic table through those two O or S atoms and contains the transition metal, disclosed, for example, in JP-A-6-136048; iminocarboxylate, thiocarboxylate and phosphine carboxylate compounds of a transition metal having a 4- to 8-membered ring chelate structure that is formed by bonding a ligand having at least one N, S or P atom and a carboxyl group (COO) to a transition metal belonging to Groups 3 to 11 of the periodic table through the N, S or P atom and the carboxyl group and contains the transition metal, disclosed, for example, in JP-T-2000-514132, JP-T-2003-535107 and JP-A-2007-77395; β-keto-phosphine, β-keto-imide and β-keto-amide compounds of a transition metal having a 4- to 8-membered ring chelate structure that is formed by bonding a ligand having at least one P or N atom and a carbonyl group (CO) to a transition metal belonging to Groups 3 to 11 of the periodic table through the P or N atom and the carbonyl group and contains the transition metal, disclosed, for example, in JP-T-2004-517933; γ-oxy-phosphine, γ-oxy-imide and γ-oxy-amide compounds of a transition metal having a 4- to 8-membered ring chelate structure that is formed by bonding a ligand having at least one P or N atom and an O atom to a transition metal belonging to Groups 3 to 11 of the periodic table through the P or N atom and the O atom and contains the transition metal, disclosed, for example, in JP-A-64-14217 and JP-T-2004-517933; a γ-sulfonato-phosphine compound of a transition metal having a 4- to 8-membered ring chelate structure that is formed by bonding a ligand having at least one P atom and a sulfonic acid residue (SO³) to a transition metal belonging to Groups 3 to 11 of the periodic table through the P atom and the sulfonic acid residue and contains the transition metal, disclosed, for example, in JP-A-6-184214, JP-A-10-195090, JP-T-2002-521534, JP-A-2007-46032 and JP-A-2007-77395; and phenoxyimine and phenoxyamine compounds of a transition metal having a 4- to 8-membered ring chelate structure that is formed by bonding a ligand having at least an N atom and a phenoxy group to a transition metal belonging to Groups 3 to 11 of the periodic table through the N atom and an O atom of the phenoxy group and contains the transition metal, disclosed, for example, in JP-A-11-315109, Chemical Communications (2003), (18), 2272-2273.

[0151] As such a non-metallocene complex catalyst, those where the center metal is Ti, Zr, Hf, which belong to Group 4B of the periodic table, V, Cr, Fe, Co, Ni or Pd exhibit high activity and are more suitably used, and those where the center metal is Ti, Zr, Hf, Fe, Ni or Pd are still more suitably used. However, with some of these post-metallocene catalysts, the ethylene-based polymer produced tends to contain a long-chain branched structure, contain a short-chain branched structure mainly consisting of a methyl branch, or have a broad molecular weight distribution and therefore, its use as the ethylene-based polymer (A) of the present invention requires special care to satisfy the conditions (A-2) to (A-4).

[0152] In the present invention, the production of the ethylene-based polymer (A) is preferably performed by contacting ethylene with the olefin polymerization catalyst of (i) to (iv) above, more preferably with (i) a Ziegler catalyst or (ii) a metallocene catalyst, and thereby polymerizing or copolymerizing the ethylene. As the olefin polymerization catalyst, a plurality of kinds may be selected from (i) to (iv) and used. At the time of performing ethylene polymerization or copolymerization, any method, for example, a liquid phase polymerization method such as slurry polymerization, solution polymerization, bulk polymerization in a liquid monomer and suspension polymerization, or a gas phase polymerization can be employed. In the case of a slurry polymerization method, either a slurry polymerization method using a pipe loop-type reactor or a slurry polymerization method using an autoclave-type reactor can be used. The industrial polymerization process is described in detail in Kazuo Matsuura and Naotaka Mikami (compilers), “Polyethylene Gijutsu Dokuhon (Polyethylene Technology Guidebook)”, page 148, 2001, Kogyo Chosakai Publishing. The polymerization method is preferably a slurry polymerization method or a gas phase polymerization method, more preferably a gas phase polymerization method.

[0153] The ethylene for use in the present invention may be an ethylene produced from a crude oil derived from a normal fossil raw material or may be a plant-derived ethylene. Also, the polyethylene produced in the present invention can be an ethylene-based polymer producing using a plant-derived ethylene. The plant-derived ethylene and the polyethylene include, for example, ethylene and polymers thereof described in JP-T-2010-511634. The plant-derived ethylene or its polymer has a property of being carbon neutral (not using a fossil raw material and not leading to an increase of carbon dioxide in the air) and can provide an environment-friendly product.

[0154] The liquid phase polymerization method is usually performed in a hydrocarbon solvent. As the hydrocarbon solvent, an inert hydrocarbon such as propane, n-butane, isobutane, n-pentane, isopentane, hexane, heptane, octane, decane, cyclohexane, benzene, toluene and xylene is used individually or as a mixture, or a liquid monomer is used. As the gas phase polymerization method, a commonly known polymerization method using a fluidized bed, a stirring bed or the like in the co-presence of an inert gas may be employed, and depending on the case, a so-called condensing mode in which a medium for removing the polymerization heat is allowed to coexist can be also employed.

[0155] The polymerization temperature is generally from 0 to 300° C., practically from 50 to 270° C., and although this may vary depending on the polymerization process employed, preferably, the polymerization temperature is from 60 to 110° C. in the slurry polymerization or suspension polymerization, from 100 to 250° C. in the solution polymerization or bulk polymerization in liquid ethylene, and from 60 to 100° C. in the gas phase polymerization method. The catalyst concentration and olefin concentration in the reactor may be an arbitrary concentration high enough for allowing the polymerization to proceed. The ethylene concentration may be from about 1 to about 10% based on the weight of the contents of the reactor in the case of slurry polymerization, suspension polymerization and solution polymerization, and in the case of gas phase polymerization, the concentration may be from 0.1 to 10 MPa in terms of the total pressure. The polymerization may be also performed by causing hydrogen to be present together, and this is commonly practiced as a method for adjusting MFR of the ethylene-based polymer (A). Hydrogen has an effect as a so-called chain transfer agent for adjusting the molecular weight in general. MFR can be adjusted to a certain extent by changing the polymerization conditions such as polymerization temperature and molar ratio of the catalyst. In order reduce the amount of the long-chain branch of the ethylene-based polymer (A), the ethylene concentration or hydrogen concentration is preferably higher.

[0156] As for the polymerization method, not only single-stage polymerization of producing an olefin-based polymer by using one reactor but also multi-stage polymerization using at least two reactors connected in series and/or in parallel for increasing the production amount or more precisely controlling the molecular weight distribution or comonomer composition distribution, can be performed. In the case of multi-stage polymerization, series multi-stage polymerization where a plurality of reactors are connected and a reaction mixture obtained by polymerization in a first-stage reactor is continuously fed in sequence to reactors of second and following stages is preferred. In the series multi-stage polymerization method, a polymerization reaction mixture in the reactor of a precedent stage is continuously discharged and transferred through a connecting pipe to reactors of subsequent and later stages. Also, the polymerization can be performed even when a so-called scavenger as a component for water removal is added to the polymerization system. As the scavenger, an organoaluminum compound such as trimethylaluminum, triethylaluminum and triisobutylaluminum, the above-described organoaluminum oxy compound, an organozinc compound, or an organomagnesium compound may be used, but an organoaluminum compound is most commonly used.

[0157] The compound (B) that is one of components constituting the polyethylene-based resin composition of the present invention satisfies all of the conditions (B-1) to (B-6) described below.

2-1. Condition (B-1)

[0158] The melt flow rate (MFR_B) of the component (B) in the present invention is from 0.01 to 1.5 g/10 min, preferably from 0.05 to 1.0 g/10 min, more preferably from 0.1 to 0.8 g/10 min.

[0159] If MFR_B is less than 0.01 g/10 min, the polyethylene-based resin composition may be inferior in the moldability, particularly in the melt flowability and spreadability, and furthermore, uniform mixing with the ethylene-based polymer (A) may be difficult, disadvantageously giving rise to production of an appearance failure such as gel, grain and fisheye or reduction in the impact strength or transparency. If MFR_B exceeds 1.5 g/10 min, the effect that the polyethylene-based resin composition or its molded product may be enhanced in the mechanical strength such as impact strength, tear strength and tensile strength as well as in the transparency may not be sufficiently exerted, and this is not preferred. In relation to MFR_A, MFR_B must further satisfy 100>MFR_A/MFR_B>1.0 so that the polyethylene-based resin composition of the present invention or its molded product can be enhanced in the mechanical strength such as impact strength, tear strength and tensile strength and in the transparency, and it is necessary to satisfy preferably 20>MFR_A/MFR_B>1.1, more preferably 15>MFR_A/MFR_B>1.2, still more preferably 10>MFR_A/MFR_B>2.0. Incidentally, MFR_B indicates a value when measured under the same conditions as in the condition (A-1).

2-2. Condition (B-2)

[0160] The density_B of the component (B) in the present invention is from 0.880 to 0.940 g/cm³, preferably from 0.891 to 0.940 g/cm³, more preferably from 0.895 to 0.925 g/cm³, still more preferably from 0.900 to 0.915 g/cm³, yet still more preferably from 0.900 to 0.910 g/cm³.

[0161] When the density_B is in this range, the polyethylene-based resin composition or its molded product is excellent in the balance between impact strength and stiffness and in the transparency. On the other hand, if the density_B is less than 0.880 g/cm³, the stiffness is reduced and when the product is a molded product having a small thickness, such as film and sheet, as well as various problems in using the product, a problem is disadvantageously brought about in the step of winding up the product or the post-processing step such as surface printing•lamination or when the product is a molded product having a large wall thickness, such as pipe and various containers, since the product is too soft and undergoes deformation, the wall thickness must be disadvantageously designed to be larger than necessary. In addition, the polymer is heavily sticky even at room temperature and difficult to handle in the blending step with the ethylene-based polymer (A), disadvantageously giving rise to product sticking of the polyethylene-based resin composition, and furthermore, the compatibility with the ethylene-based polymer (A) may be reduced to deteriorate the impact strength or transparency due to phase separation. Also, if the density_B exceeds 0.940 g/cm³, the impact strength or transparency is deteriorated and this is not preferred.

[0162] In relation to the density_A, the density_B preferably satisfies 1.070>density_A/density_B>0.990 so that the polyethylene-based resin composition of the present invention or its molded product can be enhanced in the mechanical strength such as impact strength, tear strength and tensile strength and in the transparency, and it is necessary to satisfy more preferably 1.059>density_A/density_B>1.000, still more preferably 1.050>density_A/density_B>1.005, yet still more preferably 1.035>density_A/density_B>1.010. Incidentally, density_B indicates a value when measured under the same conditions as in the condition (A-2).

2-3. Condition (B-3)

[0163] The ratio ([Mw/Mn]_B) between weight average molecular weight (Mw) and number average molecular weight (Mn) of the component (B) in the present invention is from 2.0 to 10.0, preferably from 2.0 to 6.0, more preferably from 2.5 to 5.6, still more preferably from 2.9 to 4.5, yet still more preferably from 3.2 to 4.0.

[0164] If [Mw/Mn]_B is less than 2.0, the polymer may be difficult to mix with the ethylene-based polymer (A) and therefore, this should be avoided. If [Mw/Mn]_B exceeds 10.0, the effect of improving the impact strength of the polyethylene-based resin composition or its molded product may be insufficient or deterioration of the transparency or susceptibility to sticking may result, and this is not preferred. Incidentally, [Mw/Mn]_B indicates a value when measured under the same conditions as in the condition (A-3).

[0165] 2-4. Condition (B-4)

[0166] The degree of strain hardening [λmax(2.0)]_B of the component (B) in the present invention is from 1.2 to 20.0, preferably from 1.2 to 10.0, more preferably from 1.7 to 8.0, still more preferably from 2.4 to 6.0, yet still more preferably 3.0 to 5.0.

[0167] If [λmax(2.0)]_B is less than 1.2, the ethylene-based polymer, polyethylene-based resin composition or its molded product may lack the flowability or melt tension and be deteriorated in the molding characteristics. If [λmax(2.0)]_B exceeds 20.0, the flowability and melt tension may be excellent, but the polyethylene-based resin composition or its molded product may be disadvantageously reduced in the impact strength or transparency. Incidentally, [λmax(2.0)]_B indicates a value when measured under the same conditions as in the condition (A-4). Furthermore, as to the relationship of [λmax(2.0)]_B and [λmax(2.0)]_A, when the ratio therebetween satisfies 20>[λmax(2.0)]_B/[λmax(2.0)]_A>1.0, the polyethylene-based resin composition of the present invention enhanced particularly in the balance between moldability and mechanical property, and this is preferred. If the ratio above is 20 or more, the moldability of the resin composition may be improved, but disadvantageously, the mechanical strength or transparency may be reduced, or uniform mixing of the ethylene-based polymer (A) and the ethylene-based polymer (B) may be difficult, leading to deterioration of the outer appearance. Also, if the ratio is 1.0 or less, the improvement of moldability of the resin composition may not be sufficiently exerted, and this is not preferred. The ratio is preferably 10>[λmax(2.0)]_B/[λmax(2.0)]_A >1.1, more preferably 5.0>[λmax(2.0)]_B/[λmax(2.0)]_A >1.5, still more preferably 4.0>[λmax(2.0)]_B/[λmax(2.0)]_A >1.8.

[0168] The effect of the elongational flow characteristics of the polyethylene on its moldability or mechanical properties of the molded product is as already described in general terms in the condition (A-4). As a result of intensive studies on a polyethylene-based resin composition with an attempt to improve the molding process bound up with the elongational flow characteristics of a polyethylene and overcome the problem in mechanical properties of a molded product by designing the long-chain branched structure as a main factor governing the elongational viscosity characteristics, it has been found that when an ethylene-based polymer (A) having a small amount of long-chain branched structure is used as a high MFR main component of the resin composition, that is, as a main component on the low molecular weight side and an ethylene-based polymer (B) having a large amount of long-chain branched structure represented by the degree of elongational strain hardening [λmax(2.0)]_B defined in the condition (B-4) is used as a low MFR main component of the resin composition, that is, as a main component on the high molecular weight side, it has been found that as well as enhancement of the molding characteristics, the polyethylene resin composition is excellent in the mechanical properties, particularly stiffness and impact strength, and furthermore, excellent in the transparency. In addition, when the long-chain branched structure of the ethylene-based polymer (B) has characteristics represented by the following condition (B-5) where the strain rate dependency of the degree of elongational strain hardening is different from that used conventionally, it has been found that the improving effect is very excellent in all of molding characteristics, mechanical properties and transparency of the polyethylene-based resin composition.

2-5. Condition (B-5)

[0169] As regards the component (B) in the present invention, the ratio [λmax(2.0)]_B/[λmax(0.1)]_B of [λmax(2.0)]_B defined in the condition (B-4) and [λmax(0.1)]_B measured similarly by setting the elongational strain rate to 0.1 (unit: 1/sec) is from 1.2 to 10.0, preferably from 1.3 to 5.0, more preferably from 1.4 to 4.0, still more preferably from 1.5 to 3.0.

[0170] If [λmax(2.0)]_B/[λmax(0.1)]_B is less than 1.2, non-uniform molten state of the ethylene-based polymer, polyethylene-based resin composition or its molded product or thermally unstable structure may result or reduction in the impact strength or deterioration of the transparency may be caused due to strength anisotropy that is attributable to the presence of a significantly elongated long-chain branched structure, and this is not preferred. If [λmax(2.0)]_B/[λmax(0.1)]_B exceeds 10.0, the melt tension and flowability during molding may be excellent, but the polyethylene-based resin composition or its molded product may be disadvantageously reduced in the impact strength or transparency.

2-6. Condition (B-6)

[0171] The component (B) in the present invention is a polymer produced by a polymerization reaction using a transition metal-containing catalyst, preferably a polymer produced by an ethylene polymerization reaction using a transition metal-containing catalyst described in detail later in 2-10. Production Method of Ethylene-Based Polymer (B) or in [V] Production Method of Ethylene-Based Polymer of the present invention, more preferably a polymer produced by a coordination anionic polymerization reaction of ethylene using a transition metal-containing catalyst.

[0172] At present, various radical polymerization initiators are well known as the ethylene polymerization catalyst not containing a transition metal, and specific examples thereof include a peroxide such as dialkyl peroxide compound, alkyl hydroperoxide compound, benzoyl peroxide and hydrogen peroxide, and an azo compound such as azobisisobutyronitrile and azobiscyclohexanecarbonitrile. An ethylene-based polymer produced by a radial polymerization reaction using such a radical polymerization initiator contains a large amount of long-chain branched structure and when used as a component of a polyethylene-based resin composition, the polymer may exert an effect of enhancing the molding characteristics or transparency, but the amount of long-chain branched structure becomes too large to disadvantageously reduce the strength of the composition or its molded product. In addition, realization of enough reducing of the MFR and the density of the ethylene-based polymer (B) or copolymerizing with a preferred α-olefin may be impossible and in turn, the strength of the composition or its molded product cannot be sufficiently increased, which is not preferred. Incidentally, even if the catalyst contains a transition metal, when the polymerization reaction proceeds substantially by radical polymerization as in a so-called redox system such as hydrogen peroxide/ferrous chloride or cerium salt/alcohol, the catalyst is not regarded as the transition metal-containing catalyst of the present invention.

2-7. Condition (B-7)

[0173] As regards the component (B) in the present invention, in addition to the conditions (B-1) to (B-6), furthermore, the branching index (g_C′) at a molecular weight of 1,000,000 as measured by a GPC measurement instrument with a differential refractometer, a viscosity detector and a light scattering detector is preferably from 0.30 to 0.70. The g_C′ value is more preferably from 0.30 to 0.59, still more preferably from 0.35 to 0.55, yet still more preferably from 0.35 to 0.50. If the g_C′ value exceeds 0.70, the moldability of the polyethylene-based resin composition may be insufficient, or the resin composition or its molded product may lack the transparency, and this is not preferred. If the g_C′ value is less than 0.30, the moldability of the polyethylene-based resin composition may be improved, but reduction of the impact strength of the molded product or deterioration of the transparency may disadvantageously result. Incidentally, in the present invention, the g_C′ value of the ethylene-based polymer or the W_C value in the next paragraph is an evaluation technique for the amount of long-chain branch, using the molecular weight distribution curve or branching index (g′) calculated from the GPC-VIS measurement described below.

2-8. Condition (B-8)

[0174] As regards the component (B) in the present invention, in addition to the conditions (B-1) to (B-7), furthermore, the content (W_C) of components having a molecular weight of 1,000,000 or more as measured by a GPC measurement instrument with a differential refractometer, a viscosity detector and a light scattering detector is preferably from 0.01 to 30.0%. The W_C value is more preferably from 0.01 to 10.0%, still more preferably from 0.02 to 8.0%, yet still more preferably from 0.05 to 6.0%, and most preferably from 0.09 to 4.0%.

[0175] If the W_C value is less than 0.01%, the polyethylene-based resin composition may be inferior in the moldability or the resin composition or its molded product may lack the transparency, and this is not preferred. If the W_C value exceeds 30.0%, the polyethylene-based resin composition may be enhanced in the melt tension out of the moldability, but the melt flowability may be excessively reduced to disadvantageously cause a problem in the production or molding of the resin composition. Furthermore, the impact strength or the transparency of the molded product may be deteriorated, and this is not preferred.

[Branched Structure Analysis by GPC-VIS]

[0176] As the GPC instrument having a differential refractometer (RI) and a viscosity detector (Viscometer), Alliance GPC V2000 manufactured by Waters was used. Also, as the light scattering detector, a multi-angle laser light scattering photometer (MALLS), DAWN-E, manufactured by Wyatt Technology was used. The detectors were connected in order of MALLS, RI and Viscometer. The mobile phase solvent was 1,2,4-trichlorobenzene (Irganox 1076 as an antioxidant was added at a concentration of 0.5 mg/mL). The flow rate was 1 mL/min. Two columns of GMHHR-H(S) HT manufactured by Tosoh Corporation were connected and used. The temperature of each of detectors in the column and the sample injection part was 140° C. The sample concentration was set to 1 mg/mL. The injection amount (sample loop volume) was 0.2175 mL. In determining the absolute molecular weight (M) obtained from MALLS, the square radius of gyration (R_g) and the intrinsic viscosity ([η]) obtained from Viscometer, the data processing software ASTRA (version 4.73.04) attached to MALLS was utilized, and computation was performed by referring to the following literatures.

[0177] 1. Developments in polymer characterization, vol. 4. Essex: Applied Science; 1984. Chapter 1.

[0178] 2. Polymer, 45, 6495-6505 (2004)

[0179] 3. Macromolecules, 33, 2424-2436 (2000)

[0180] 4. Macromolecules, 33, 6945-6952 (2000)

[Calculation of Branching Index (g_C′), etc.]

[0181] The branching index (g′) is calculated as a ratio (ηbranch/ηlin) between the intrinsic viscosity (ηbranch) obtained by measuring the sample by Viscometer and the intrinsic viscosity (ηlin) obtained by separately measuring a linear polymer.

[0182] When a long-chain branch is introduced into a polymer molecule, the radius of gyration becomes small as compared with a molecule of a linear polymer having the same molecular weight, and when the radius of gyration becomes small, the intrinsic viscosity decreases. Therefore, along with introduction of a long-chain branch, the ratio (ηbranch/ηlin) of the intrinsic viscosity (ηbranch) of a branched polymer to the intrinsic viscosity (ηlin) of a linear polymer having the same molecular weight becomes small. Accordingly, it is meant that when the branching index (g′=ηbranch/ηlin) takes a value smaller than 1, a branch is introduced and as the value becomes smaller, the amount of long-chain branch introduced is increased. Particularly, in the present invention, the content percentage (%) of components having a molecular weight of 1,000,000 or more in terms of the absolute molecular weight obtained from MALLS to the amount of all components measured by RI is calculated as the content (W_C) of components having a molecular weight of 1,000,000 or more, and the above-described g′ at a molecular weight of 1,000,000 in terms of the absolute molecular weight obtained from MALLS is calculated as g_C′.

[0183] FIG. 4(a) and FIG. 4(b) shown an example of the analysis results by GPC-VIS above. FIG. 4(a) shows a molecular weight distribution curve measured based on the molecular weight (M) obtained from MALLS and the concentration obtained from RI, and FIG. 4(b) shows a branching index (g′) at the molecular weight (M). Here, as the linear polymer, a linear polyethylene, Standard Reference Material 1475a (National Institute of Standards & Technology), was used.

2-9. Composition of Ethylene-Based Polymer (B)

[0184] As for the composition of the component (B) in the present invention, the description in 1-5. Composition of Ethylene-Based Polymer (A) above can apply as-is except for the ratio between ethylene and α-olefin, and with respect to the same portions, description is omitted.

[0185] The ethylene-based polymer (B) of the present invention is preferably a copolymer of ethylene and the α-olefin described above in 1-5. and most preferably a copolymer with hexene-1 and octene-1. The ratio of ethylene and the α-olefin in the ethylene-based polymer (B) of the present invention is from about 75 to 99.5 wt % of ethylene and from about 0.5 to 25 wt % of α-olefin, preferably from about 78 to 97 wt % of ethylene and from about 3 to 22 wt % of α-olefin, more preferably from about 80 to 96 wt % of ethylene and from about 4 to 20 wt % of α-olefin, still more preferably from about 82 to 95 wt % of ethylene and from about 5 to 18 wt % of α-olefin. When the ethylene content is in this range, the polyethylene-based resin composition or its molded product has good balance between stiffness and impact strength and is excellent also in the transparency. In the case of using the above-described dienes, the dienes must be of course used in the range where the long-chain branched structure satisfies the conditions (B-4) and (B-5).

2-10. Production Method of Ethylene-Based Polymer (B)

[0186] As for the production method of the ethylene-based polymer (B) in the present invention, the description in 1-6. Production Method of Ethylene-Based Polymer (A) above can apply as-is except that selection of an olefin polymerization catalyst appropriate to provide for a long-chain branched structure corresponding to the conditions (B-4) and (B-5) to the ethylene-based polymer (B) must be taken care of, and with respect to the same portions, description is omitted.

[0187] The transition metal-containing olefin polymerization catalyst suitable for the production of the ethylene-based polymer (B) in the present invention and satisfying the profitability at the industrial level is, similarly to the ethylene-based polymer(A), appropriately selected from the above-described (i) Ziegler catalyst, (ii) metallocene catalyst, (iii) Phillips catalyst and (iv) post-metallocene catalyst and used.

[0188] The catalyst used for the production of the ethylene-based polymer (B) in the present invention is more suitably (i) a Ziegler catalyst, (ii) a metallocene catalyst or (iv) a post-metallocene catalyst, still more suitably (i) a Ziegler catalyst or (ii) a metallocene catalyst. Among others, (ii) a metallocene catalyst produces an ethylene-based polymer having a narrow molecular weight distribution or a narrow copolymerization composition distribution as compared with other catalysts and therefore, is preferred from the standpoint of enhancing the mechanical properties, transparency, anti-sticking performance, heat seal performance and the like of the polyethylene-based resin composition or its molded product. Of course, in the case of selecting (iv) a post-metallocene catalyst capable of exerting the same performances from the standpoint above, use of the catalyst is preferred.

[0189] Out of the characteristics which the ethylene-based polymer (B) in the present invention must satisfy, the particularly important characteristics represented by the condition (B-4) and the condition (B-5), preferably the condition (B-4), the condition (B-5) and the condition (B-7), are considered to be attributable to a characteristic long-chain branched structure that is understood to contain a fairly large amount of a shortish branch structure sufficiently developed to an extent of enabling branches to intertwine with each other at a level where an elongational strain hardening behavior is observed.

[0190] In general, an ethylene-based polymer having a long-chain branch is an ethylene-based polymer having a long branching structure (long-chain branch) in the polyethylene molecule and is contrasted with an ethylene homopolymer or ethylene.α-olefin copolymer having a normal short-chain branch (sometimes referred to as straight chain polyethylene). For producing such an ethylene-based polymer having a long-chain branch, various methods have been heretofore attempted, and examples thereof include a method of directly copolymerizing ethylene and an α-olefin by using a recent Ziegler catalyst or metallocene catalyst, and a method of copolymerizing ethylene and a previously produced macromonomer to introduce a long-chain branch. Also, an ethylene-based polymer producing using a catalyst called a Phillips catalyst where the center metal is a hexavalent chromium element, is supposed to contain a small amount of a long-chain branched structure. As for the literature specifically describing the production of an ethylene-based polymer having a long-chain branched structure, the method using a recent Ziegler catalyst is described, for example, in JP-A-60-090203 and JP-10-298234. In these methods, the long-chain branched structure of the ethylene-based polymer can be adjusted by appropriately selecting the kind and amount of the organoaluminum compound, the kind of the catalyst or the polymerization conditions so as to control the quality and amount of the long-chain branch. As for the production using a metallocene-based catalyst, the method using a complex having a bridged biscyclopentadienyl ligand is described, for example, in JP-A-2002-544296 and JP-A-2005-507961; the method using a complex having an indenyl ligand is described, for example, in JP-A-2-276807, JP-A-2002-308933, JP-A-2004-292772, JP-A-8-311121, JP-A-8-311260 and JP-A-8-48711; the method using a catalyst obtained by combining a non-MAO-modified particle with a complex having a bridged bisindenyl ligand is described, for example, in JP-A-2004-292772; the method using a constrained geometry complex catalyst is described, for example, in JP-A-6-306121; and the method using a combination of a benzindenyl ligand-containing complex with another low-molecular-weight polyethylene-producing complex is described, for example, in JP-A-2006-2098.

[0191] In these methods, the quality and amount of the long-chain branch can be controlled by appropriately selecting the kind of the complex, the catalyst preparation conditions or the polymerization conditions. Also, a method of introducing a long-chain branch into a polyethylene chain by using dienes as a comonomer and copolymerizing it with ethylene is disclosed, for example, in JP-A-10-512600, and a method of introducing a long-chain branch into a polyethylene chain by utilizing a chain transfer reagent as T-reagent is disclosed, for example, in JP-T-2008-505222. In these methods, the quality and amount of the long-chain branch can be controlled by controlling the kind or amount of the dienes or chain transfer agent or appropriately selecting the kind of the catalyst or the polymerization conditions. Furthermore, a method where a macromonomer is previously produced by using a specific metallocene-based catalyst and then the macromonomer is copolymerized with ethylene, thereby introducing a long-chain branch into a polyethylene chain, is disclosed, for example, in JP-A-7-252311, JP-A-8-502303, International Publication No. 95-11931, JP-T-2001-511215 and JP-A-2006-321991. In these methods, the quality and amount of the long-chain branch can be controlled by appropriately selecting the kind of the complex, the catalyst preparation conditions, the polymerization conditions, or the amount or molecular weight of the macromonomer. The index indicative of such an ethylene-based polymer having a long-chain branch is generally expressed by various measurement techniques and the like, for example, by the melt flow rate ratio (MFR ratio; see, for example, Japanese Patent 2,571,280), the melt tension (MT; see, for example, Japanese Patent 3,425,719), the presence or absence of rising of elongational viscosity (strain hardening) (see, for example, Japanese Patent 4,190,638), and the activation energy (see, for example, JP-A-7-062031). The resin that is commercially available in practice includes, for example, trade name: AFFINITY (registered trademark) FM1570 (produced by Dow Chemical), and trade name: Excellen GMH (registered trademark) (produced by Sumitomo Chemical Co., Ltd.).

[0192] However, not all of ethylene-based polymers having a long-chain branched structure produce by these methods are suited for the ethylene-based polymer (B) as a constituent component of the polyethylene-based resin composition of the present invention. The present inventors have found that selection of the specific ethylene-based polymer (B) leads to greatly different results in the molding characteristics, mechanical strength and transparency of the polyethylene-based composition or a molded product of the composition, and in addition to the selection of a long-chain branched structure suitable for the present invention, only when an ethylene-based polymer (B) of which MFR, density and molecular weight distribution conditions are suitably designed as described above is used as a constituent component of the polyethylene-based composition, the present invention has been accomplished.

[0193] The ethylene-based polymer having a long-chain branched structure, which can be produced by the conventional technique, includes, as described above, a polymer produced using a Ziegler catalyst, a polymer produced using a complex having a bridged biscyclopentadienyl ligand, a polymer produced using a bridged bisindenyl ligand, a polymer produced using a catalyst obtained by combining a bridged bisindenyl ligand-containing complex with a non-MAO-modified particle, a polymer produced using a constrained geometry complex catalyst, a polymer produced using a combination of a benzindenyl ligand-containing complex with another low-molecular-weight polyethylene-producing complex, a polymer in which a long-chain branch is introduced into a polyethylene chain by using dienes as a comonomer and copolymerizing it with ethylene, a polymer in which a long-chain branch is introduced into a polyethylene chain by utilizing a chain transfer reagent as T-reagent, and a polymer produced by a method where a macromonomer is previously produced by using a specific metallocene-based catalyst and then the macromonomer is copolymerized with ethylene, thereby introducing a long-chain branch into a polyethylene chain.

[0194] However, when the ethylene-based copolymer produced using a Ziegler catalyst is used as the ethylene-based polymer (B) in the present invention, the molecular weight distribution or copolymerization composition distribution may be broadened to make the polyethylene-based resin composition or its molded product be insufficient in the impact strength or transparency, or the polymer may be heavily sticky due to a large amount of low crystalline components, and therefore, this is not preferred. In addition, with the catalyst above, only a small amount of an elongated long-chain branched structure can be produced, failing in sufficiently enhancing the impact strength or transparency. When an ethylene-based copolymer produced using a bridged biscyclopentadienyl ligand-containing complex or a bridged bisindenyl ligand-containing complex is used, the molecular weight distribution tends to be broadened, making the polyethylene-based resin composition or its molded product be insufficient in the impact strength or transparency, or the chain length of the long-chain branch tends to become long, failing in sufficiently enhancing the impact resistance or transparency. When an ethylene-based copolymer produced using a catalyst obtained by combining a bridged bisindenyl ligand-containing complex with a non-MAO-modified particle is used, the molecular weight distribution tends to be more broadened than in the case of using an MAO promoter and in turn, the polyethylene-based resin composition or its molded product may be insufficient in the impact strength or transparency. For example, Excellen GMH that is a commercial product produced using the catalyst above in practice has a wide molecular weight distribution and an elongated long-chain branch and lacks in the number of branches, as a result, the effect of improving the moldability may be low or the impact strength or transparency may not be sufficiently enhanced. When an ethylene-based copolymer produced using a constrained geometry complex catalyst is used, for example, AFFINITY (for example, FM1570) that is a commercial product produced using the catalyst above in practice has a long chain length of the long-chain branch and lacks in the number of branches, as a result, the effect of improving the moldability may be low or the impact strength or transparency may not be sufficiently enhanced. As the case now stands, none of these methods are preferred as the production method of the ethylene-based polymer (B) in the present invention.

[0195] The ethylene-based copolymer produced using a combination of a benzindenyl ligand-containing complex with another low-molecular-weight polyethylene-producing complex is thought to have some possibility of realizing a long-chain branched structure required of the ethylene-based polymer (B) in the present invention, but for the production of a long-chain branched structure, the polymerization conditions may be limited to a low hydrogen concentration, the catalyst conditions such as proportion of a complex used or the polymerization conditions must be further studied so as to avoid broadening of the molecular weight, or studies on the setting of MFR or density of the ethylene-based polymer (B) or the ethylene-based polymer (A) combined are required. Furthermore, in order to realize a long-chain branched structure appropriate as the ethylene-based polymer (B) in the present invention by the method of copolymerizing dienes or the method utilizing a chain transfer reagent, the kind of the dienes, chain transfer agent or polymerization catalyst used or the polymerization conditions must be further studied. In addition, it is considered that problems such as contamination (odor, coloring, deterioration) of the polymer by the residual diene or residual chain transfer agent must be solved. Also, in order to realize a long-chain branched structure appropriate as the ethylene-based polymer (B) in the present invention by the method of producing a macromonomer and copolymerizing it with ethylene to thereby introduce a long-chain branch into the polyethylene chain, for example, the kind of the polymerization catalyst used, the polymerization conditions, and the control of molecular weight, density and copolymerization ratio of the produced macromer must be further studied and in addition, since a residual macromer remains as a low-molecular-weight polymer in the polymer or in the polyethylene-based resin composition containing the polymer as one component, the molecular weight distribution or the copolymerization composition distribution tends to be broadened, leaving high possibility that the impact strength or transparency of the polyethylene-based resin composition or its molded product becomes insufficient, which reveals that the polymer is not preferred enough. For these reasons, the ethylene-based polymer (B) tends to have a longish chain length of the long-chain branch and in turn, the impact strength and transparency may not be sufficiently enhanced. Also, it is considered that problems such as contamination (odor, coloring, deterioration) of the polymer must be solved.

[0196] That is, as a result of intensive studies to attain the object of the present invention, with respect to the olefin polymerization catalyst capable of producing a long-chain branched structure suitable as the ethylene-based polymer (B) of the present invention, the present inventors have reached, as an example, a method where a complex having a bridged (cyclopentadienyl)(indenyl) ligand or the like that has been discovered recently is used as an essential catalyst component (for example, JP-A-2011-137146 and [V] Production Method of Ethylene-Based Polymer of the Present Invention in this description); as another example, a method where a complex having a benzindenyl ligand or the like is used as a catalyst component (for example, JP-A-2006-2098); and, as still another example, a method where a catalyst using a mixture of a metallocene complex, i.e., a complex having a bridged bis(indenyl) ligand, a bridged bis(azulenyl) ligand or a bridged bis(cyclopentadienyl) ligand, and a borane or borate compound as a compound for producing a cationic metallocene compound together with an organoaluminum oxy compound, is used.

[0197] The olefin polymerization catalyst containing, as an essential component, a complex having a bridged (cyclopentadienyl)(indenyl) ligand or the like capable of producing a long-chain branched structure suitable as the ethylene-based polymer (B) of the present invention contains the following component (a-1) and component (b) and, if desired, further contains the component (c):

[0198] component (a-1): a metallocene compound represented by formula (a-1-1),

[0199] component (b): a compound capable of reacting with the metallocene compound of the component (a-1) to produce a cationic metallocene compound, and

[0200] component (c): a microparticle support.

i) Component (a-1)

[0201] The component (a-1) is a metallocene compound represented by the following formula (a-1-1):

[0202]
[in formula (a-1-1), M represents any one transition metal of Ti, Zr and Hf; each of X¹ and X² independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; each of Q¹ and Q² independently represents a carbon atom, a silicon atom or a germanium atom; each R¹ independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and at least two members out of four R¹ may combine to form a ring together with Q¹ and Q²; m is 0 or 1 and when m is 0, Q¹ is bonded directly to the conjugated 5-membered ring including R² and R³; each R² independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20 and even when the plurality of R² are a hydrocarbon group or the like, unlike R⁴, these R² do not form a ring together with the carbon atoms to which R² are bonded; R³ represents a saturated or unsaturated divalent hydrocarbon group having a carbon number of 4 or 5 for forming a condensed ring with the 5-membered ring to which R³ is bonded; R⁴ is an atom or a group bonded to a carbon atom of R³ and each independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20; n represents an integer of 0 to 10 and when n is 2 or more, at least two R⁴ may form a ring together with the carbon atoms to which R⁴ are bonded; and each R⁵ independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen atom-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20 and even when the plurality of R⁵ are a hydrocarbon group or the like, unlike R⁴, these R⁵ do not form a ring together with the carbon atoms to which R⁵ are bonded].

[0203] In formula (a-1-1), M of the metallocene compound represents Ti, Zr or Hf. M is preferably Zr or Hf and from the standpoint that the polymerization activity is high, M is more preferably Zr. In the present invention, this preference order of center metal species applies in all descriptions of metallocene complexes below.

[0204] Each of X¹ and X² independently includes, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a methoxymethyl group, an ethoxymethyl group, an n-propoxymethyl group, an i-propoxymethyl group, an n-butoxymethyl group, an i-butoxymethyl group, a tert-butoxymethyl group, a methoxyethyl group, an ethoxyethyl group, an acetyl group, a 1-oxopropyl group, a 1-oxo-n-butyl group, a 2-methyl-1-oxopropyl group, a 2,2-dimethyl-1-oxo-propyl group, a phenylacetyl group, a diphenylacetyl group, a benzoyl group, a 2-methoxyphenyl group, a 3-methoxyphenyl group, a 4-methoxyphenyl group, a 2-furyl group, a 2-tetrahydrofuryl group, a dimethylaminomethyl group, a diethylaminomethyl group, a di-i-propylaminomethyl group, a bis(dimethylamino)methyl group, a bis(di-i-propylamino)methyl group, a (dimethylamino)(phenyl)methyl group, a methylimino group, an ethylimino group, a 1-(methylimino)ethyl group, a 1-(phenylimino)ethyl group, a 1-[(phenylmethyl)imino]ethyl group, an ethoxy group, an n-propoxy group, an i-propoxy group, an n-butoxy group, an i-butoxy group, a tert-butoxy group, a phenoxy group, a dimethylamino group, a diethylamino group, a di-n-propylamino group, a di-i-propylamino group, a di-n-butylamino group, a di-i-butylamino group, a di-tert-butylamino group, and a diphenylamino group.

[0205] Specific preferred examples of X¹ and X² include a chlorine atom, a bromine atom, a methyl group, an n-butyl group, an i-butyl group, a methoxy group, an ethoxy group, an i-propoxy group, an n-butoxy group, a phenoxy group, a dimethylamino group, and a di-i-propylamino group. Among these specific examples, a chlorine atom, a methyl group and a dimethylamino group are more preferred.

[0206] Each of Q¹ and Q² independently represents a carbon atom, a silicon atom or a germanium atom and is preferably a carbon atom or a silicon atom.

[0207] Each R¹ independently includes, for example, a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, and a phenyl group. In the case where R¹ forms a ring together with Q¹ and Q², examples include a cyclobutylidene group, a cyclopentylidene group, a cyclohexylidene group, a silacyclobutyl group, a silacyclopentyl group, and a silacyclohexyl group.

[0208] When Q¹ or/and Q² are a carbon atom, specific preferred examples of R¹ include a hydrogen atom, a methyl group, an ethyl group, a phenyl group and a cyclobutylidene group, and when Q¹ or/and Q² are a silicon atom, specific preferred examples include a methyl group, an ethyl group, a phenyl group and a silacyclobutyl group.

[0209] Each R² independently includes, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, and a phenyldimethylsilyl group.

[0210] Out of two R², at least one is preferably a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20, because the polymerization activity becomes high in particular. Also, R² on the 2-position is preferably a hydrogen atom, because the characteristics of the long-chain branched structure are particularly improved and in turn, the moldability is excellent.

[0211] Specific preferred examples of R², each independently, include a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a 2-methylfuryl group, and a trimethylsilyl group.

[0212] Among these specific examples, a hydrogen atom, a methyl group, an n-butyl group, a tert-butyl group, a phenyl group and a trimethylsilyl group are more preferred, and a hydrogen atom, a methyl group and a phenyl group are still more preferred.

[0213] Specific examples of the condensed cyclopentadienyl structure formed by R³ and a cyclopentadienyl moiety to which R³ is bonded, include the following partial structures (I) to (VI).

[0214] Among these specific examples, (I), (III) and (VI) are preferred. Also, R⁴ may be substituted on these partial structures (I) to (VI).

[0215]

[0216] The substituent R⁴ includes, in addition to a hydrogen atom, for example, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 4-tert-butylphenyl group, a 3,5-dimethylphenyl group, a 3,5-di-tert-butylphenyl group, a naphthyl group, an anthracenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 2,6-dichloro-4-trimethylsilylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, and a phenyldimethylsilyl group.

[0217] In the case where two or more R⁴ form a ring together with the carbon atoms to which R⁴ are bonded, examples include a benz[e]indenyl group, a benz[f]indenyl group, a 6,7-dihydroindacenyl group, a 5,5,7,7-tetramethyl-6,7-dihydroindacenyl group, a 5,6,7,8-tetrahydro-benz[f]indenyl group, and a 5,6,7,8-tetrahydro-5,5,8,8-tetramethyl-benz[f]indenyl group.

[0218] Specific preferred examples of R⁴ include a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a naphthyl group, and a trimethylsilyl group.

[0219] Each R⁵ independently includes, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, and a phenyldimethylsilyl group.

[0220] Out of four R⁵, at least one is preferably a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20, because the polymerization activity is particularly increased. Also, R⁵ on the 2-position and 5-position are preferably a hydrogen atom, because the characteristics of the long-chain branched structure are particularly improved and in turn, the moldability is excellent.

[0221] Specific preferred examples of R⁵ include a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a 2-methylfuryl group, and a trimethylsilyl group.

[0222] Among these specific examples, a hydrogen atom, a methyl group, an n-butyl group, a tert-butyl group, a phenyl group and a trimethylsilyl group are more preferred, and a hydrogen atom, a methyl group, a tert-butyl group and a phenyl group are still more preferred.

[0223] In formula (a-1-1), m is 0 or 1 and when m is 0, Q¹ is bonded directly to the conjugated 5-membered ring including R² and R³. Furthermore, n represents an integer of 0 to 10 and when n is 2 or more, at least two R⁴ may form a ring together with the carbon atoms to which R⁴ are bonded.

[0224] The metallocene compound of the component (a-1) is preferably a compound represented by the following formula (a-1-2), more preferably a compound represented by the following formula (a-1-3):

[0225]

[0226] In the metallocene compounds represented by formulae (a-1-2) and (a-1-3), for X¹, X², Q, R¹, R², R⁴ and R⁵, the same structures as the atoms and groups described in the metallocene compound represented by formula (a-1-1) may be selected.

[0227] Specific examples of the metallocene compound of the component (a-1) are shown in Tables a-1 to a-4 below, but the present invention is not limited thereto. In Tables a-1 to a-4, Cp stands for a cyclopentadienyl group, Ind stands for an indenyl group, Me stands for a methyl group, Ph stands for a phenyl group, Et stands for an ethyl group, nPr stands for an n-propyl group, nBu stands for an n-butyl group, nC5 stands for an n-pentyl group, nC6 stands for an n-hexyl group, Bz stands for a benzyl group, and Azu stands or an azulenyl group.

[0228]

TABLE a-1
(i) Bridged Cp(Ind)Zr Type
				Ind
	No.	Q	Cp Substituent	Substituent	X
	1a	Me2Si	—	—	Cl
	2a	Me2Si	—	—	Me
	3a	Me2Si	—	—	Ph
	4a	Me2C	—	—	Cl
	5a	silacyclobutyl	—	—	Cl
	6a	silacyclopentyl	—	—	Cl
	7a	silacyclohexyl	—	—	Cl
	8a	cyclobutylidene	—	—	Cl
	9a	cyclopentylidene	—	—	Cl
	10a	cyclohexylidene	—	—	Cl

[0229]

TABLE a-2
(ii) Bridged Cp(3-substituted Ind)Zr Type
				Ind
	No.	Q	Cp Substituent	Substituent	X
	11a	Me2Si	—	3-Me	Cl
	12a	Me2Si	—	3-Me	Me
	13a	Me2C	—	3-Me	Cl
	14a	Me2Si	—	3-Et	Cl
	15a	Me2C	—	3-Et	Cl
	16a	Me2Si	—	3-nPr	Cl
	17a	Me2C	—	3-nPr	Cl
	18a	Me2Si	—	3-iPr	Cl
	19a	Me2C	—	3-iPr	Cl
	20a	Me2Si	—	3-nBu	Cl
	21a	Me2C	—	3-nBu	Cl
	22a	Me2Si	—	3-tBu	Cl
	23a	cyclobutylidene	—	3-tBu	Cl
	24a	Me2Si	—	3-tBu	Me
	25a	Me2C	—	3-tBu	Cl
	26a	Me2Si	—	3-nC5	Cl
	27a	Me2Si	—	3-nC6	Cl
	28a	Me2Si	—	3-cycC6	Cl
	29a	Me2Si	—	3-Ph	Cl
	30a	Me2Si	—	3-Bz	Cl
	31a	Me2Si	—	3-tolyl	Cl
	32a	Me2Si	—	3-TMS	Cl
	33a	Me2Si	—	3-ClPh	Cl
	34a	Me2Si	—	3-FPh	Cl
	35a	Me2Si	—	4-Me	Cl
	36a	Me2Si	—	5-Me	Cl
	37a	Me2Si	—	6-Me	Cl
	38a	Me2Si	—	3,4-Me2	Cl
	39a	Me2Si	—	3-tBu-4-Me	Cl
	40a	Me2Si	—	4-Ph	Cl

[0230]

TABLE a-3
(ii) Bridged Cp (3-Substituted Ind)Zr Type (continued)
No.	Q	Cp Substituent	Ind Substituent	X
41a	Me2Ge	—	—	Cl
42a	Me2Ge	—	3-Me	Cl
43a	Me2Ge	—	3-Et	Cl
44a	Me2Ge	—	3-iPr	Cl
45a	Me2Ge	—	3-nBu	Cl
46a	Me2Ge	—	3-tBu	Cl
47a	Et2Si	—	—	Cl
48a	Et2Si	—	3-Me	Cl
49a	Et2Si	—	3-Et	Cl
50a	Et2Si	—	3-iPr	Cl
51a	Et2Si	—	3-nBu	Cl
52a	Et2Si	—	3-tBu	Cl
53a	nBu2Si	—	—	Cl
54a	nBu2Si	—	3-Me	Cl
55a	nBu2Si	—	3-Et	Cl
56a	nBu2Si	—	3-iPr	Cl
57a	nBu2Si	—	3-nBu	Cl
58a	nBu2Si	—	3-tBu	Cl
59a	Ph2Si	—	—	Cl
60a	Ph2C	—	—	Cl
61a	Ph2Si	—	3-Me	Cl
62a	Ph2Si	—	3-Et	Cl
63a	Ph2Si	—	3-iPr	Cl
64a	Ph2Si	—	3-nBu	Cl
65a	Ph2Si	—	3-tBu	Cl
66a	Me2Si	—	benz[e]	Cl
67a	Me2Si	—	dibenzo	Cl
68a	Me2Si	—	azulenyl	Cl
69a	Me2Si	—	4-Me-Azu	Cl
70a	Me2Si	—	4-Ph-Azu	Cl
71a	Me2Si	—	5,6-Me2	Cl
72a	Me2Si	—	benz[f]	Cl
73a	Me2Si	—	6,7-dihydroindacenyl	Cl
74a	Me2Si	—	5,5,7,7-Me4-6,7-dihydroindacenyl	Cl
75a	Me2Si	—	5,6,7,8-H4-benz[f]	Cl
76a	Me2Si	—	5,6,7,8-H4-5,5,8,8-Me4-benz[f]	Cl

[0231]

TABLE a-4
(iv) Bridged(4-Substituted Cp)(3-Substituted
Ind)Zr Type
No.	Q	Cp Substituent	Ind Substituent	X
77a	Me2Si	4-tBu	3-Me	Cl
78a	Me2Si	4-tBu	3-tBu	Cl
79a	Me2Si	4-tBu	3-tBu	Me
80a	Me2Si	4-tBu	2-Me	Cl
81a	Me2Si	4-tBu	2-Me-4Ph	Cl
82a	Me2C	2-Me	3-tBu	Cl
83a	Me2Si	4-tBu	—	Cl
84a	Me2Si	2,3-Me2	3-tBu	Cl
85a	Me2Si	2,3,4-Me3	—	Cl
86a	Me2Si	2,3,4,5-Me4	—	Cl
87a	Me2Si	4-tBu	—	Me
88a	Me2Si	4-tBu	4,5,6,7-H4	Cl
89a	Me2Si	4-tBu	Azu	Cl
90a	Me2Si	4-tBu	2-(2-Me-Furyl)	Cl
91a	Me2Si	2-(2-Me-Furyl)	3-Me	Cl
92a	Me2Si	4-TMS	—	Cl
93a	Me2Si	4-(2-Br—Et)	—	Cl

[0232] The metallocene compound also includes, for example, compounds where zirconium of the compounds above is replaced by titanium or hafnium.

[0233] Furthermore, in using these metallocene compounds as the component (a-1), two or more thereof may be also used.

[0234] Among specific compounds exemplified above, preferred metallocene compounds as the component (a-1) include the followings.

[0235] That is, preferred examples include dimethylsilylene-(cyclopentadienyl)(indenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(indenyl)zirconium dimethyl, isopropylidene(cyclopentadienyl)(indenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-methylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-methylindenyl)zirconium dimethyl, isopropylidene(cyclopentadienyl)(3-methylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-n-butylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-phenylindenyl)zirconium dichloride, isopropylidene(cyclopentadienyl)(3-n-butylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-tert-butylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-tert-butylindenyl)zirconium dimethyl, dimethylsilylene(cyclopentadienyl)(4-phenylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(benz[e]indenyl)zirconium dichloride, isopropylidene(cyclopentadienyl)(3-tert-butylindenyl)zirconium dichloride, cyclobutylidene(cyclopentadienyl)(3-tert-butylindenyl)zirconium dichloride, dimethylgermirene(cyclopentadienyl)(indenyl)zirconium dichloride, diphenylsilylene-(cyclopentadienyl)(indenyl)zirconium dichloride, diphenylmethylene(cyclopentadienyl)(indenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(azulenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(3-methylindenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(3-tert-butylindenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(3-tert-butylindenyl)zirconium dimethyl, dimethylsilylene(4-tert-butylcyclopentadienyl)(4-phenylindenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(indenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(indenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(indenyl)zirconium dimethyl, dimethylsilylene(4-tert-butylcyclopentadienyl)(4,5,6,7-tetrahydroindenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(azulenyl)zirconium dichloride, and compounds where zirconium of the compounds above is replaced by titanium or hafnium.

[0236] Among specific examples exemplified above, more preferred examples of the metallocene compound as the component (a-1) include the followings:

[0237] dimethylsilylene(cyclopentadienyl)(indenyl)zirconium dichloride, isopropylidene(cyclopentadienyl)(indenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-methylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-phenylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(4-phenylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(benz[e]indenyl)zirconium dichloride, isopropylidene(cyclopentadienyl)(3-methylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(3-tert-butylindenyl)zirconium dichloride, isopropylidene(cyclopentadienyl)(3-tert-butylindenyl)zirconium dichloride, dimethylgremirene(cyclopentadienyl)(indenyl)zirconium dichloride, cyclobutylidene(cyclopentadienyl)(3-tert-butylindenyl)zirconium dichloride, dimethylsilylene(cyclopentadienyl)(indenyl)hafnium dichloride, dimethylsilylene(cyclopentadienyl)(3-methylindenyl)hafnium dichloride, dimethylsilylene(cyclopentadienyl)(3-tert-butylindenyl)hafnium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(indenyl)zirconium dichloride, dimethylsilylene(4-tert-butylcyclopentadienyl)(indenyl)zirconium dichloride, and dimethylsilylene(4-tert-butylcyclopentadienyl)(indenyl)zirconium dimethyl.

ii) Component (b)

[0238] The olefin polymerization catalyst recited as an example of the olefin polymerization catalyst containing, as an essential component, a complex having a bridged (cyclopentadienyl)(indenyl) ligand or the like capable of producing a long-chain branched structure suitable as the ethylene-based polymer (B) of the present invention contains, in addition to the component (a-1), a compound capable of reacting with the metallocene compound of the component (a-1) (component (a-1); hereinafter, sometimes simply referred to as “a”) to produce a cationic metallocene compound (component (b); hereinafter, sometimes simply referred to as “b”).

[0239] One of the compound (b) capable of reacting with the metallocene compound (a) to produce a cationic metallocene compound is an organoaluminum oxy compound.

[0240] The organoaluminum oxy compound has an Al—O—Al bond in the molecule, and the number of bonds is usually from 1 to 100, preferably from 1 to 50. Such an organoaluminum oxy compound is a product obtained usually by reacting an organoaluminum compound and water.

[0241] Incidentally, out of the organoaluminum oxy compounds, the compound obtained by reacting an alkyl aluminum and water is usually called an aluminoxane, and methylaluminoxane (encompasses those substantially composed of methylaluminoxane (MAO)) is particularly suitable as the organoaluminum oxy compound.

[0242] Other specific examples of the compound (b) capable of reacting with the metallocene compound (a) to form a cationic metallocene compound include a borane compound and a borate compound.

[0243] Specific examples of the borane compound include triphenylborane, tri(o-tolyl)borane, tri(p-tolyl)borane, tri(m-tolyl)borane, tri(o-fluorophenyl)borane, tris(p-fluorophenyl)borane, tris(m-fluorophenyl)borane, tris(2,5-difluorophenyl)borane, tris(3,5-difluorophenyl)borane, tris(4-trifluoromethylphenyl)borane, tris(3,5-ditrifluoromethylphenyl)borane, tris(2,6-ditrifluoromethylphenyl)borane, tris(pentafluorophenyl)borane, tris(perfluoronaphthyl)borane, tris(perfluorobiphenyl), tris(perfluoroanthryl)borane, and tris(perfluorobinaphthyl)borane.

[0244] Also, the borate compound is specifically, as a first example, a compound represented by the following formula (b-1):
[L¹−H]⁺[BR⁶R⁷X⁴X⁵]  formula (b-1)

[0245] In formula (b-1), L¹ is a neutral Lewis base, H is a hydrogen atom, and [L¹-H] is a Broensted acid such as ammonium, anilinium and phosphonium.

[0246] Examples of the ammonium include a trialkyl-substituted ammonium such as trimethylammonium, triethylammonium, tripropylammonium, tributylammonium and tri(n-butyl)ammonium, and a dialkylammonium such as di(n-propyl)ammonium and dicyclohexylammonium.

[0247] Examples of the anilinium include an N,N-dialkyl anilinium such as N,N-dimethylanilinium, N,N-diethylanilinium and N,N-2,4,6-pentamethylanilinium.

[0248] Furthermore, the phosphonium includes a triarylphosphonium and a trialkylarylphosphonium, such as triphenylphosphonium, tributylphosphonium, tri(methylphenyl)phosphonium and tri(dimethylphenyl)phosphonium.

[0249] In formula (b-1), R⁶ and R⁷ are, each independently, the same or different aromatic or substituted aromatic hydrocarbon group having a carbon number of 6 to 20, preferably from 6 to 16, and may be connected to each other by a bridging group. The substituent of the substituted aromatic hydrocarbon group is preferably an alkyl group typified, for example, by a methyl group, an ethyl group, a propyl group and an isopropyl group, or a halogen atom such as fluorine, chlorine, bromine and iodine.

[0250] Each of X⁴ and X⁵ is independently a hydride group, a halide group, a hydrocarbon group having from 1 to 20 carbon atoms, or a substituted hydrocarbon group having from 1 to 20 carbon atoms, in which one or more hydrogen atoms are substituted for by a halogen atom.

[0251] Specific examples of the compound represented by formula (b-1) include tributylammoniumtetra(pentafluorophenyl)borate, tributylammoniumtetra(2,6-ditrifluoromethylphenyl)borate, tributylammoniumtetra(3,5-ditrifluoromethylphenyl)borate, tributylammoniumtetra(2,6-difluorophenyl)borate, tributylammoniumtetra(perfluoronaphthyl)borate, dimethylaniliniumtetra(pentafluorophenyl)borate, dimethylaniliniumtetra(2,6-ditrifluoromethylphenyl)borate, dimethylaniliniumtetra(3,5-ditrifluoromethylphenyl)borate, dimethylaniliniumtetra(2,6-difluorophenyl)borate, dimethylaniliniumtetra(perfluoronaphthyl)borate, triphenylphosphoniumtetra(pentafluorophenyl)borate, triphenylphosphoniumtetra(2,6-ditrifluoromethylphenyl)borate, triphenylphosphoniumtetra(3,5-ditrifluoromethylphenyl)borate, triphenylphosphoniumtetra(2,6-difluorophenyl)borate, triphenylphosphoniumtetra(perfluoronaphthyl)borate, trimethylammoniumtetra(2,6-ditrifluoromethylphenyl)borate, triethylammoniumtetra(pentafluorophenyl)borate, triethylammoniumtetra(2,6-ditrifluoromethylphenyl)borate, triethylammoniumtetra(perfluoronaphthyl)borate, tripropylammoniumtetra(pentafluorophenyl)borate, tripropylammoniumtetra(2,6-ditrifluoromethylphenyl)borate, tripropylammoniumtetra(perfluoronaphthyl)borate, di(1-propyl)ammoniumtetra(pentafluorophenyl)borate, and dicyclohexylammoniumtetraphenylborate.

[0252] Among these, preferred are tributylammoniumtetra(pentafluorophenyl)borate, tributylammoniumtetra(2,6-ditrifluoromethylphenyl)borate, tributylammoniumtetra(3,5-ditrifluoromethylphenyl)borate, tributylammoniumtetra(perfluoronaphthyl)borate, dimethylaniliniumtetra(pentafluorophenyl)borate, dimethylanilinumtetra(2,6-ditrifluoromethylphenyl)borate, dimethylaniliniumtetra(3,5-ditrifluoromethylphenyl)borate and dimethylaniliniumtetra(perfluoronaphthyl)borate.

[0253] A second example of the borate compound is represented by the following formula (b-2):
[L²]⁺[BR⁶R⁷X⁴X⁵]⁻  formula (b-2)

[0254] In formula (b-2), L² includes, for example, a carbo-cation, a methyl cation, an ethyl cation, a propyl cation, an isopropyl cation, a butyl cation, an isobutyl cation, a tert-butyl cation, a pentyl cation, a tropinium cation, a benzyl cation, a trityl cation, a sodium cation, and a proton.

[0255] R⁶, R⁷, X⁴ and X^s have the same definitions as those in formula (b-1).

[0256] Specific examples of the compound above include trityltetraphenylborate, trityltetra(o-tolyl)borate, trityltetra(p-tolyl)borate, trityltetra(m-tolyl)borate, trityltetra(o-fluorophenyl)borate, trityltetra(p-fluorophenyl)borate, trityltetra(m-fluorophenyl)borate, trityltetra(3,5-difluorophenyl)borate, trityltetra(pentafluorophenyl)borate, trityltetra(2,6-ditrifluoromethylphenyl)borate, trityltetra(3,5-ditrifluoromethylphenyl)borate, trityltetra(perfluoronaphthyl)borate, tropiniumtetraphenylborate, tropiniumtetra(o-tolyl)borate, tropiniumtetra(p-tolyl)borate, tropiniumtetra(m-tolyl)borate, tropiniumtetra(o-fluorophenyl)borate, tropiniumtetra(p-fluorophenyl)borate, tropiniumtetra(m-fluorophenyl)borate, tropiniumtetra(3,5-difluorophenyl)borate, tropiniumtetra(pentafluorophenyl)borate, tropiniumtetra(2,6-ditrifluoromethylphenyl)borate, tropiniumtetra(3,5-ditrifluoromethylphenyl)borate, tropiniumtetra(perfluoronaphthyl)borate, NaBPh₄, NaB(o-CH₃-Ph)₄, NaB(p-CH₃-Ph)₄, NaB(m-CH₃-Ph)₄, NaB(o-F-Ph)₄, NaB(p-F-Ph)₄, NaB(m-F-Ph)₄, NaB(3,5-F₂-Ph)₄, NaB(C₆F₅)₄, NaB(2,6-(CF₃)₂-Ph)₄, NaB(3,5-(CF₃)₂-Ph)₄, NaB(C₁₀F₇)₄, H⁺BPh₄.2-diethyl ether, H⁺B(3,5-F₂-Ph)₄.2-diethyl ether, H⁺B(C₆F₅)₄⁻.2-diethyl ether, H⁺B(2,6-(CF₃)₂-Ph)₄.2-diethyl ether, H⁺B(3,5-(CF₃)₂-Ph)₄.2-diethyl ether, and H⁺B(C₁₀H₇)₄.2-diethyl ether.

[0257] Among these, preferred are trityltetra(pentafluorophenyl)borate, trityltetra(2,6-ditrifluoromethylphenyl)borate, trityltetra(3,5-ditrifluoromethylphenyl)borate, trityltetra(perfluoronaphthyl)borate, tropiniumtetra(pentafluorophenyl)borate, tropiniumtetra(2,6-ditrifluoromethylphenyl)borate, tropiniumtetra(3,5-ditrifluoromethylphenyl)borate, tropiniumtetra(perfluoronaphthyl)borate, NaB(C₆F₅)₄, NaB(2,6-(CF₃)₂-Ph)₄, NaB(3,5-(CF₃)₂-Ph)₄, NaB(C₁₀F₇)₄, H⁺B(C₆F₅)₄⁻.2-diethyl ether, H⁺B(2,6-(CF₃)₂-Ph)₄.2-diethyl ether, H⁺B(3,5-(CF₃)₂-Ph)₄.2-diethyl ether and H⁺B(C₁₀H₇)₄.2-diethyl ether.

[0258] Among these, more preferred are trityltetra(pentafluorophenyl)borate, trityltetra(2,6-ditrifluoromethylphenyl)borate, tropiniumtetra(pentafluorophenyl)borate, tropiniumtetra(2,6-ditrifluoromethylphenyl)borate, NaB(C₆F₅)₄, NaB(2,6-(CF₃)₂-Ph)₄, H⁺B(C₆F₅)₄⁻.2-diethyl ether, H⁺B(2,6-(CF₃)₂-Ph)₄.2-diethyl ether, H⁺B(3,5-(CF₃)₂-Ph)₄.2-diethyl ether and H⁺B(C₁₀H₇)₄.2-diethyl ether.

[0259] When a borane compound or a borate compound is used as the catalyst component (b), the polymerization activity or copolymerizability increases and therefore, productivity of an ethylene-based polymer having a long-chain branch is enhanced.

[0260] Other specific examples of the compound (b) capable of reacting with a metallocene compound (a) to produce a cationic metallocene compound include a clay mineral, a layered silicate compound, and a chemically treated solid oxide.

[0261] In addition, a mixture of the above-described organoaluminum oxy compound and the above-described borane compound or borate compound may be also used as the component (b), and in order to more enhance the long-chain branched structure required of the ethylene-based polymer (B) in the present invention, it is preferred to use the borane compound or borate compound in combination with the organoaluminum oxy compound. Furthermore, as for the borane compound or borate compound, two or more compounds may be mixed and used.

iii) Component (c)

[0262] The olefin polymerization catalyst recited as an example of the olefin polymerization catalyst containing, as an essential component, a complex having a bridged (cyclopentadienyl)(indenyl) ligand or the like capable of producing a long-chain branched structure suitable as the ethylene-based polymer (B) of the present invention preferably contains a microparticle support (component (c); hereinafter, sometimes simply referred to as “c”).

[0263] The microparticle support as the component (c) includes an inorganic support, a particulate polymer support, and a mixture thereof. As the inorganic support, a metal, a metallic oxide, a metallic chloride, a metallic carbonate, a carbonaceous substance, or a mixture thereof can be used.

[0264] Preferred examples of the metal that can be used for the inorganic support include iron, aluminum, and nickel.

[0265] The metallic oxide includes a single oxide or a composite oxide of elements belonging to Groups 1 to 14 of the periodic table, and examples thereof include various natural or synthetic, single or composite oxides such as SiO₂, Al₂O₃, MgO, CaO, B₂O₃, TiO₂, ZrO₂, Fe₂O₃, Al₂O₃.MgO, Al₂O₃.CaO, Al₂O₃.SiO₂, Al₂O₃.MgO.CaO, Al₂O₃.MgO.SiO₂, Al₂O₃.CuO, Al₂O₃.Fe₂O₃, Al₂O₃.NiO and SiO₂.MgO.

[0266] Incidentally, these formulae are not a molecular formula but indicate only a composition, and the structure and component ratio of the composite oxide for use in the present invention are not particularly limited.

[0267] Also, the metallic oxide for use in the present invention may have absorbed a small amount of water or may contain a small amount of impurities.

[0268] As the metallic chloride, for example, a chloride of an alkali metal or an alkaline earth metal is preferred, and specifically, MgCl₂, CaCl₂ and the like are suited in particular.

[0269] As the metallic carbonate, a carbonate of an alkali metal or an alkaline earth metal is preferred, and specific examples thereof include magnesium carbonate, calcium carbonate, and barium carbonate.

[0270] The carbonaceous substance includes, for example, carbon black and activated carbon.

[0271] All of these inorganic supports can be suitably used in the present invention, but among others, use of a metallic oxide, silica, alumina or the like is preferred.

[0272] A specific example of the olefin polymerization catalyst containing, as an essential component, a benzindenyl ligand or the like capable of producing a long-chain branched structure suitable as the ethylene-based polymer (B) of the present invention is an olefin polymerization catalyst comprising the following component (a-2), the component (b), and the preferred component (c).

iv) Component (a-2)

[0273] The component (a-2) is a metallocene compound having one or more, preferably two or more, more preferably three, benzindenyl ligands are represented by the following formula (a-2-1):

[0274]

[0275] Here, each of the substituents R⁸ to R¹³ is independently a hydrocarbon group having a carbon number of 1 to 30, or a trialkyl silicon group having a hydrocarbon substituent with a carbon number of 1 to 30. Specific examples of the hydrocarbon group include an alkyl group such as methyl group, ethyl group, propyl group, butyl group, pentyl group, hexyl group and cyclohexyl group; an alkenyl group such as vinyl group and allyl group; an aryl group such as phenyl group, dimethylphenyl group, diethylphenyl group, dipropylphenyl group, dibutylphenyl group, trimethylphenyl group, triethylphenyl group, tripropylphenyl group, tributylphenyl group, biphenyl group, naphthyl group and anthryl group; an arylalkyl group such as trityl group, phenethyl group, benzhydryl group, phenylpropyl group, phenylbutyl group and neophyl group; and an arylalkenyl group such as styryl group. These groups may have a branch. Also, out of the substituents R⁸ to R¹³, adjacent two substituents may form a ring together with the carbon atoms to which the substituents are bonded. In addition, when the component (a-2) has three cyclopentadienyl skeleton-containing ligands including the benzindenyl ligand, a metallocene complex where two or more members of those ligands are bridged, for example, by the same ethylene bridging group or dimethylsilylene groups as the bridging group composed of Q¹, Q² and R¹ defined in formula (a-1-1), such as hydrocarbon group, silylene group and substituted silylene group, is also effective. Incidentally, the center transition metal and the group (auxiliary ligand) except for a cyclopentadienyl skeleton-containing ligand bonded to the center transition metal are the same as those of M, X¹ and X² defined in formula (a-1-1), such as hydrocarbon group, alkoxyl group, halogen atom and hydrogen atom.

[0276] Specific examples of the component (a-2) where, for example, the center transition metal is Zr, are shown in Tables a-5 and a-6 below. In Tables a-5 and a-6, Cp stands for a cyclopentadienyl group, Ind stands for an indenyl group, Bzind stands for a benzindenyl group, Dbi stands for a dibenzindenyl group, Me stands for a methyl group, and Bu stands for a butyl group.

[0277]

TABLE a-5
ABCDZr
	No.	A	B	C	D
	95a	BzInd	BzInd	Cl	Cl
	96a	BzInd	BzInd	Br	Br
	97a	BzInd	BzInd	Me	Me
	98a	Dbi	Dbi	Cl	Cl
	99a	Dbi	Dbi	Br	Br
	100a	Dbi	Dbi	Me	Me
	101a	BzInd	BzInd	BzInd	H
	102a	Dbi	Dbi	Dbi	H
	103a	BzInd	BzInd	Cp	H
	104a	BzInd	BzInd	1,3-Me2-Cp	H
	105a	BzInd	BzInd	1-Bu-3-Me-Cp	H
	106a	BzInd	BzInd	Ind	H
	107a	BzInd	Ind	Ind	H
	108a	Dbi	Dbi	Cp	H
	109a	Dbi	Cp	Cp	H
	110a	Dbi	Dbi	Ind	H
	111a	Dbi	Ind	Ind	H
	112a	BzInd	BzInd	Dbi	H
	113a	BzInd	Dbi	Dbi	H
	114a	BzInd	Dbi	Cp	H
	115a	BzInd	Dbi	Ind	H

[0278]

TABLE a-6
		No.	A1	A2	A3	A4	A5
		116a	Et	Ind	Ind	BzInd	H
		117a	Et	Ind	Ind	Dbi	H
		118a	Me2Si	Cp	Cp	BzInd	H
		119a	Me2Si	Cp	Cp	DBi	H
		120a	Me2Si	Cp	Ind	Dbi	H
		121a	Et	BzInd	BzInd	Cp	H
		122a	Et	BzInd	BzInd	Ind	H

[0279] Specific preferred examples of the component (a-2) are Bzind₃ZrH, Dbi₃ZrH, Bzind₂ CpZrH, Bzind₂(1,3-Me₂Cp)ZrH, Bzind₂(1-Bu-3-MeCp)ZrH, Bzind₂IndZrH, BzindInd₂ZrH, Dbi₂ CpZrH, DbiCp₂ZrH, Dbi₂IndZrH, DbiInd₂ZrH, Bzind₂ DbiZrH, BzindDbi₂ZrH, BzindDbiCpZrH, BzindDbiIndZrH, Et(Ind)₂BzindZrH, Et(Ind)₂ DbiZrH, Me₂SiCp₂BzindZrH, Me₂SiCp₂ DbiZrH, Me₂Si(Cp)(Ind)DbiZrH, Et(Bzind)₂ CpZrH and Et(Bzind)₂IndZrH, and more preferred specific examples are Bzind₃ZrH, Dbi₃ZrH, Bzind₂ CpZrH, Bzind₂(1,3-Me₂Cp)ZrH, Bzind₂(1-Bu-3-MeCp)ZrH, Bzind₂IndZrH, BzindInd₂ZrH, Dbi₂ CpZrH, DbiCp₂ZrH, Dbi₂IndZrH, DbiInd₂ZrH, Bzind₂ DbiZrH, BzindDbi₂ZrH, BzindDbiCpZrH and BzindDbiIndZrH.

[0280] As described above, together with the component (a-2), the organoaluminum oxy compound above or the like is used as the component (b), and also in this case, the borane compound or borate compound is preferably used in combination with the organoaluminum oxy compound so as to more enhance the characteristics of the long-chain branched structure required of the ethylene-based polymer (B) in the present invention. Similarly, it is also preferred to contain the component (c) in addition to the component (a-2) and the component (b).

[0281] A specific example of the olefin polymerization catalyst containing, as an essential component, a mixture of a complex having a bridged bis(indenyl), bridged bis(azulenyl) or bridged bis(cyclopentadienyl) ligand capable of producing a long-chain branched structure as the ethylene-based polymer (B) of the present invention and a borane or borate compound as a compound for producing a cationic metallocene compound together with an organoaluminum oxy compound is an olefin polymerization catalyst comprising the following component (a-3), a mixture of an organoaluminum oxy compound and a borane or borate compound described in the component (b), and the preferred component (c).

[0282] Here, the complex having a bridged bis(indenyl) ligand, a bridged bis(azulenyl) ligand or a bridged bis(cyclopentadienyl) ligand (referred to as components (a-3-1), (a-3-2) and (a-3-3), respectively) indicates a complex having a basic skeleton where same or different two cyclopentadienyl rings or same or different two indenyl rings as represented by formula [2] in the classification of metallocene compounds described above in the paragraph of 1-6. (ii) Metallocene Catalyst are bridged by a bridging group Q¹. The substituent which can be substituted on the cyclopentadienyl ring, indenyl ring, azulenyl ring or bridging group Q¹ has a high degree of freedom as long as it does not inhibit the basic skeleton structure, and a metallocene complex or the like having a heteroatom-containing monocyclic or polycyclic heteroaromatic group as a substituent on a ligand of a conjugated 5-membered ring structure described, for example, in JP-T-2002-535339 may be also suitably used.

[0283]
[wherein each of A³ and A⁴ represents a ligand having a conjugated 5-membered ring structure (A³ and A⁴ may be the same or different in the same compound), Q¹ represents a bonding group for bridging two conjugated 5-membered ring ligands at arbitrary positions, M represents a metal atom selected from Group 4 of the periodic table, and each of X and Y independently represents a hydrogen atom, a halogen atom, a hydrocarbon group, an alkoxy group, an amino group, a phosphorus-containing hydrocarbon group or a silicon-containing hydrocarbon group, which is bonded to M].

[0284] As specific examples of the complex having a bridged bis(indenyl) ligand of the component (a-3-1), when the center transition is Zr:

[0285] (I) out of the compounds represented by formula [2], compounds where the bonding group Q has, for example, a structure recited below, are shown in Tables a-7 to a-9. In Tables a-7 to a-9, Ind stands for an indenyl group, and TMS stands for a trimethylsilyl group.

[0286] (I-1) When Q¹ is an alkylene group, the complex includes, for example, the compounds shown in Table a-7 below.

[0287]

TABLE a-7
Q1 = alkylene group
No.	Q1	A3	A4	X	Y
123a	CH2	Ind	Ind	Cl	Cl
124a	Et	Ind	Ind	Cl	Cl
125a	Et	Ind	Ind	Cl	H
126a	Et	Ind	Ind	Cl	Me
127a	Et	Ind	Ind	Cl	OMe
128a	Et	Ind	Ind	OEt	OEt
129a	Et	Ind	Ind	Me	Me
130a	Et	H4Ind	H4Ind	Cl	Cl
131a	Et	2-Me-Ind	2-Me-Ind	Cl	Cl
132a	Et	2-Et-Ind	2-Et-Ind	Cl	Cl
133a	Et	2,4-Me2-Ind	2,4-Me2-Ind	Cl	Cl
134a	Et	4-Ind	4-Ind	Cl	Cl
135a	Et	2-(2-(5-	2-(2-(5-	Cl	Cl
		MeFuryl))Ind	MeFuryl))Ind
136a	Et	2-(2-(5-	2-(2-(5-	Cl	Cl
		MeFuryl))-4-	MeFuryl))-4-
		Ph-Ind	Ph-Ind
137a	Et	4-(2,7-Me2-Ind)	4-(2,7-Me2-Ind)	Cl	Cl
138a	Et	2-(2-(5-	2-(2-(5-	Cl	Cl
		tBuFuryl)-4-	tBuFuryl)-4-
		Ph-Ind)	Ph-Ind)
139a	Et	2-(2-(5-	Ind	Cl	Cl
		tBuFuryl)-4-
		Ph-Ind)
140a	Et	4-Ph-Ind	4-Ph-Ind	Cl	Cl
141a	Me2C	Ind	Ind	Cl	Cl
142a	Et	Ind	Ind	Cl	H

[0288] (I-2) When Q¹ is a silylene group, the complex includes, for example, the compounds shown in Table a-8 below. In Table a-8, Ind stands for an indenyl group, BenInd stands for a benzindenyl group, PhInd stands for a phenylindenyl group, and TMSPh stands for a trimethylsilylphenyl group.

[0289]

TABLE 8
a-8
Q1 = silylene group
No.	Q1	A3	A4	X	Y
143a	Me2Si	Ind	Ind	Cl	Cl
144a	Me2Si	4,5,6,7-H4Ind	4,5,6,7-H4Ind	Cl	Cl
145a	Me2Si	2-Me-Ind	2-Me-Ind	Cl	Cl
146a	Me2Si	2,4-Me2-Ind	2,4-Me2-Ind	Cl	Cl
147a	Me2Si	2-Me-4,5,6,7-H4Ind	2-Me-4,5,6,7-H4Ind	Cl	Cl
148a	Me2Si	2-Me-4,5-BenInd	2-Me-4,5-BenInd	Cl	Cl
149a	Me2Si	2-Me-4-Ph-Ind	2-Me-4-Ph-Ind	Cl	Cl
150a	Me2Si	2-Me-4,4-Me2-4,5,6,7-H4-4-	2-Me-4,4-Me2-4,5,6,7-H4-4-	Cl	Cl
		silaindenyl	silaindenyl
151a	Me2Si	4-(2-Ph-Ind)	4-(2-Ph-Ind)	Cl	Cl
152a	Me2Si	4-(2-tBuInd)	4-(2-tBuInd)	Cl	Cl
153a	Me2Si	4-(2-Ph-3-MeInd)	4-(2-Ph-3-MeInd)	Cl	Cl
154a	PhMeSi	Ind	Ind	Cl	Cl
155a	PhMeSi	4,5,6,7-H4Ind	4,5,6,7-H4Ind	Cl	Cl
156a	Ph2Si	Ind	Ind	Cl	Cl
157a	tetramethyl-	Ind	Ind	Cl	Cl
	disilylene
158a	Me2Si	2-(2-(5-MeFuryl))-4-PhInd	2-(2-(5-MeFuryl))-4-PhInd	Cl	Cl
159a	Me2Si	2-(2-(5-TMSFuryl))-4-PhInd	2-(2-(5-TMSFuryl))-4-PhInd	Cl	Cl
160a	Me2Si	2-(2-(5-PhFuryl)-4-PhInd)	2-(2-(5-PhFuryl)-4-PhInd)	Cl	Cl
161a	Me2Si	2-(2-(5-Methienyl))-4-	2-(2-(5-Methienyl))-4-	Cl	Cl
		PhInd	PhInd
162a	Me2Si	2-(2-(4,5-Me2Furyl))-4-	2-(2-(4,5-Me2Furyl))-4-	Cl	Cl
		PhInd	PhInd
163a	Me2Si	2-(2-BenFuryl)-4-PhInd	2-(2-BenFuryl)-4-PhInd	Cl	Cl
164a	Me2Si	2-(2-BenThienyl)-4-(4-	2-(2-BenThienyl)-4-(4-	Cl	Cl
		TMSPh)-Ind	TMSPh)-Ind
165a	Me2Si	2-(2-(5-TMSFuryl))-4-(2-	2-(2-(5-TMSFuryl))-4-(2-	Cl	Cl
		Naph)-Ind	Naph)-Ind
166a	PhMeSi	2-(2-(5-MeFuryl))-4-PhInd	2-(2-(5-MeFuryl))-4-PhInd	Cl	Cl
167a	Me2Si	2-(2-(5-MeFuryl))-4-PhInd	2-(2-(5-MeFuryl))-4-(4-	Cl	Cl
			tBuPh)-Ind
168a	Me2Si	2-(2-(5-MeFuryl))-4-PhInd	2-(2-(5-MeFuryl))-4-(4-	Cl	Cl
			TMSPh)-Ind
169a	Me2Si	2-(2-(5-MeFuryl))-4-(4-	2-(2-(5-MeFuryl))-4-(4-	Cl	Cl
		tBuPh)-Ind	TMSPh)-Ind

[0290] (I-3) When Q¹ is a hydrocarbon group containing germanium, phosphorus, nitrogen, boron or aluminum, the complex includes, for example, the compounds shown in Table a-9 below. In Table a-9, Ind stands for an indenyl group, PhInd stands for a phenylindenyl group, and TMSPh stands for a trimethylsilylphenyl group.

[0291]

TABLE a-9
No.	Q1	A3	A4	X	Y
170a	Me2Ge	Ind	Ind	Cl	Cl
171a	MeAl	Ind	Ind	Cl	Cl
172a	PhAl	Ind	Ind	Cl	Cl
173a	PhP	Ind	Ind	Cl	Cl
174a	EtB	Ind	Ind	Cl	Cl
175a	PhN	Ind	Ind	Cl	Cl
176a	Me2Ge	2-(2-(5-	2-(2-(5-	Cl	Cl
		MeFuryl))-4-	MeFuryl))-4-
		PhInd	PhInd
177a	MeB	2-(2-(5-	2-(2-(5-	Cl	Cl
		MeFuryl))-4-	MeFuryl))-4-
		(4-TMSPh)-Ind	(4-TMSPh)-Ind

[0292] As specific examples of the complex having a bridged bis(azulenyl) ligand of the component (a-3-2), when the center transition is Zr:

[0293] (II) out of the compounds represented by formula [2], compounds where the bonding group Q¹ has, for example, a structure recited below, are shown in Tables a-10 to a-12.

[0294] (II-1) When Q¹ is an alkylene group, the complex includes, for example, the compounds shown in Table a-10 below. In Tables a-10 to a-12, tBuPh stands for tributylphenyl group, TMSPh stands for a trimethylsilylphenyl group, NaPh stands for a naphthyl group, BiPh stands for a biphenyl group, Azu stands for an azulenyl group, and CIPh stands for a chlorophenyl group.

[0295]

TABLE a-10
Q1 = alkylene group
No.	Q1	A3	A4	X	Y
178a	CH2	2-Et-4-(3-Cl-4-tBuPh)-4-	2-Et-4-(3-Cl-4-tBuPh)-4-	Cl	Cl
		HAzu	HAzu
179a	Et	2-Me-4-(3-Me-4-tBuPh)-4-	2-Me-4-(3-Me-4-tBuPh)-4-	Cl	Cl
		HAzu	HAzu
180a	Et	2-Me-4-(3-Cl-4-TMSPh)-4-	2-Me-4-(3-Cl-4-TMSPh)-4-	Cl	H
		HAzu	HAzu
181a	Et	2-Me-4-(2-Naph)-4-HAzu	2-Me-4-(2-Naph)-4-HAzu	Cl	Me
182a	Et	2-Me-4-(2-F-4-BiPh)-4-HAzu	2-Me-4-(2-F-4-BiPh)-4-	Cl	OMe
			HAzu
183a	Et	2-Me-4-(2-Cl-4-BiPh)-4-	2-Me-4-(2-Cl-4-BiPh)-4-	OEt	OEt
		HAzu	HAzu
184a	Et	2-Me-4-(9-phenanthryl)-4-	2-Me-4-(9-phenanthryl)-4-	Me	Me
		HAzu	HAzu

[0296] (II-2) When Q¹ is a silylene group, the complex includes, for example, the compounds shown in Table a-11 below.

[0297]

TABLE a-11
Q1 = silylene group
No.	Q1	A3	A4	X	Y
185a	Me2Si	2-Me-4-Ph-4-HAzu	2-Me-4-Ph-4-HAzu	Cl	Cl
186a	Me2Si	2-Me-4-(4-ClPh)-4-HAzu	2-Me-4-(4-ClPh)-4-HAzu	Cl	Cl
187a	Me2Si	2-Me-4-(4-tBuPh)-4-HAzu	2-Me-4-(4-tBuPh)-4-HAzu	Cl	Cl
188a	Me2Si	2-Me-4-(4-TMSPh)-4-HAzu	2-Me-4-(4-TMSPh)-4-HAzu	Cl	Cl
189a	Me2Si	2-Me-4-(3-Cl-4-tBuPh)-4-HAzu	2-Me-4-(3-Cl-4-tBuPh)-4-HAzu	Cl	Cl
190a	Me2Si	2-Me-4-(3-Me-4-TMSPh)-4-HAzu	2-Me-4-(3-Me-4-TMSPh)-4-HAzu	Cl	Cl
191a	Me2Si	2-Me-4-(1-Naph)-4-HAzu	2-Me-4-(1-Naph)-4-HAzu	Cl	Cl
192a	Me2Si	2-Et-4-(4-ClPh)-4-HAzu	2-Et-4-(4-ClPh)-4-HAzu	Cl	Cl
193a	Me2Si	2-Me-4-(4-Cl-2-Naph)-4-HAzu	2-Me-4-(4-Cl-2-Naph)-4-HAzu	Cl	Cl
194a	Me2Si	2-nPr-4-(3-Cl-4-TMSPh)-4-HAzu	2-nPr-4-(3-Cl-4-TMSPh)-4-HAzu	Cl	Cl

[0298] (II-3) When Q¹ is a hydrocarbon group containing germanium, phosphorus, nitrogen, boron or aluminum, the complex includes, for example, the compounds shown in Table a-12 below.

[0299]

TABLE a-12
No.	Q1	A3	A4	X	Y
195a	Me2Ge	2-Me-4-(2-F-4-	2-Me-4-(2-F-4-	Cl	Cl
		BiPh)-4-HAzu	BiPh)-4-HAzu
196a	PhAl	2-Me-4-(2-F-4-	2-Me-4-(2-F-4-	Cl	Cl
		BiPh)-4-HAzu	BiPh)-4-HAzu
197a	Me2Ge	2-Me-4-(4-tBuPh)-	2-Me-4-(4-tBuPh)-	Cl	Cl
		4-HAzu	4-HAzu

[0300] As specific examples of the complex having a bridged bis(cyclopentadienyl) ligand of the component (a-3-3), when the center transition is Zr:

[0301] (III) out of the compounds represented by formula [2], compounds where the bonding group Q¹ has, for example, a structure recited below, are shown in Tables a-13 to a-16. In Tables a-13 to a-16, Cp stands for a cyclopentadienyl group, TMS stands for trimethylsilyl, and Flu stands for fluorenyl.

[0302] (III-1) When Q¹ is an alkylene group, the complex includes, for example, the compounds shown in Table a-13 below.

[0303]

TABLE a-13
Q1 = alkylene group
No.	Q1	A3	A4	X	Y
198a	Et	2,4-Me2Cp	3′,5′-MeCp	Cl	Cl
199a	Et	2-Me-4-tBuCp	3′-tBu-5′-MeCp	Cl	Cl
200a	Et	2,3,5-Me3Cp	2′,4′,5′-Me3Cp	Cl	Cl
201a	Me2C	2,4-Me2Cp	3′,5′-Me2Cp	Cl	Cl
202a	CH2	Cp	3,4-Me2Cp	Cl	Cl
203a	CH2	Cp	3,4-Me2Cp	Cl	H
204a	CH2	Cp	3,4-Me2Cp	Me	Me
205a	CH2	Cp	3,4-Me2Cp	Ph	Ph
206a	CH2	Cp	TMSCp	Cl	Cl
207a	CH2	Cp	Me4Cp	Cl	Cl
208a	Me2C	Cp	3,4-Me2Cp	Cl	Cl
209a	Me2C	Cp	Me4Cp	Cl	Cl
210a	Me2C	Cp	Flu	Cl	Cl
211a	Me2C	2-MeCp	Flu	Cl	Cl
212a	Me2C	3-tBuCp	Flu	Cl	Cl
213a	Me2C	2,5-Me2Cp	3′,4′-Me2Cp	Cl	Cl
214a	Me2C	2,5-Me2Cp	Flu	Cl	Cl
215a	Et	Cp	3,5-Me2Cp	Cl	Cl
216a	Et	Cp	Flu	Cl	Cl
217a	Et	2,5-Me2Cp	Flu	Cl	Cl
218a	Et	2,5-Et2Cp	Flu	Cl	Cl
219a	Ph2C	Cp	3,4-Et2Cp	Cl	Cl
220a	cyclo-	Cp	Flu	Cl	Cl
	hexyl-
	idene
221a	cyclo-	2,5-Me2Cp	3′,4′-Me2Cp	Cl	Cl
	hexyl-
	idene
222a	Et	2-(2-(5-MeFuryl))Cp	2-(2-(5-MeFuryl))Cp	Cl	Cl
223a	Et	2-(2-(5-MeFuryl))-	2-(2-(5-MeFuryl))-	Cl	Cl
		4-PhCp	4-PhCp
224a	Et	2-(2-(5-tBuFuryl))Cp	2-(2-(5-tBuFuryl))Cp	Cl	Cl
225a	Et	2-(2-(5-tBuFuryl))-	Cp	Cl	Cl
		4-PhCp

[0304] (III-2) When Q¹ is a silylene group, the complex includes, for example, the compounds shown in Tables a-14 and a-15 below.

[0305]

TABLE a-14
Q1 = silylene group
No.	Q	A3	A4	X	Y
227a	Me2Si	2,4-Me2Cp	3′,5′-MeCp	Cl	Cl
228a	PhMeSi	2,4-Me2Cp	3′,5′-MeCp	Cl	Cl
229a	PhMeSi	2,3,5-Me3Cp	2′,4′,5′-Me3Cp	Cl	Cl
230a	PhMeSi	Me4Cp	Me4Cp	Cl	Cl
231a	tetramethyl-	Cp	Cp	Cl	Cl
	disilylene
232a	Me2Si	Cp	3,4-Me2Cp	Cl	Cl
233a	Me2Si	Cp	Me3Cp	Cl	Cl
234a	Me2Si	Cp	Me4Cp	Cl	Cl
235a	Me2Si	Cp	3,4-Et2Cp	Cl	Cl
236a	Me2Si	Cp	Et3Cp	Cl	Cl
237a	Me2Si	Cp	Me4Cp	Cl	Cl
238a	Me2Si	Cp	Flu	Cl	Cl
239a	Me2Si	3-tBuCp	Flu	Cl	Cl
240a	Me2Si	Cp	2,7-tBu2Flu	Cl	Cl
241a	Me2Si	Cp	H8Flu	Cl	Cl
242a	Me2Si	2-MeCp	Flu	Cl	Cl
243a	Me2Si	2,5-Me2Cp	Flu	Cl	Cl
244a	Me2Si	2-EtCp	Flu	Cl	Cl
245a	Me2Si	2,5-Et2Cp	Flu	Cl	Cl
246a	Et2Si	2-MeCp	2′,7′-tBu2Flu	Cl	Cl
247a	Me2Si	2,5-Me2Cp	2′,7′-tBu2Flu	Cl	Cl
248a	Me2Si	2-EtCp	2′,7′-tBu2Flu	Cl	Cl
249a	Me2Si	Et2Cp	2′,7′-tBu2Flu	Cl	Cl
250a	Me2Si	Et2Cp	H8Flu	Cl	Cl
251a	Me2Si	Me2Cp	H8Flu	Cl	Cl
252a	Me2Si	EtCp	H8Flu	Cl	Cl
253a	Me2Si	Et2Cp	H8Flu	Cl	Cl

[0306]

TABLE a-15
Q1 = silylene group (continued)
No.	Q	A3	A4	X	Y
254a	Me2Si	2-(2-(5-tBuFuryl))Cp	2-(2-(5-tBuFuryl))Cp	Cl	Cl
255a	Me2Si	2-(2-(5-TMSFuryl))Cp	2-(2-(5-TMSFuryl))Cp	Cl	Cl
256a	Me2Si	2-(2-(5-PhFuryl))Cp	2-(2-(5-PhFuryl))Cp	Cl	Cl
257a	Me2Si	2-(2-(5-MeThienyl))Cp	2-(2-(5-MeThienyl))Cp	Cl	Cl
258a	Me2Si	2-(2-(4,5-Me2Furyl))Cp	2-(2-(4,5-Me2Furyl))Cp	Cl	Cl
259a	Me2Si	2-(2-BenFuryl)Cp	2-(2-BenFuryl)Cp	Cl	Cl
260a	Me2Si	2-(2-BenThienyl)-4-(4-TMSPh)Cp	2-(2-BenThienyl)-4-(4-TMSPh)Cp	Cl	Cl
261a	Me2Si	2-(2-(5-TMSFuryl))Cp	2-(2-(5-TMSFuryl))Cp	Cl	Cl
262a	PhMeSi	2-(2-(5-MeFuryl))Cp	2-(2-(5-MeFuryl))Cp	Cl	Cl
263a	Me2Si	2-(2-(5-MeFuryl))Cp	Cp	Cl	Cl
264a	Me2Si	2-(2-(5-MeFuryl))-4-PhCp	2-(2-(5-MeFuryl))Cp	Cl	Cl
265a	Me2Si	2-(2-(5-MeFuryl))Cp	3-MeCp	Cl	Cl

[0307] (III-3) When Q¹ is a hydrocarbon group containing germanium, phosphorus, nitrogen, boron or aluminum, the complex includes, for example, the compounds shown in Table a-16 below.

[0308]

TABLE a-16
No.	Q1	A3	A4	X	Y
266a	Me2Ge	Cp	Flu	Cl	Cl
267a	PhN	Cp	Flu	Cl	Cl
268a	Me2Ge	2-(2-(5-MeFuryl))Cp	2-(2-(5-MeFuryl))Cp	Cl	Cl
269a	MeB	2-(2-(5-MeFuryl))-4-	2-(2-(5-MeFuryl))-4-	Cl	Cl
		TMSCp	TMSCp

[0309] Thanks to a catalyst where a mixture of an organoaluminum oxy compound and a borane compound or the like is combined with a complex having a bridged bis(indenyl) ligand, a bridged bis(azulenyl) ligand or a bridged bis(cyclopentadienyl) ligand, which is defined by the compounds above, a long-chain branched structure suitable as the ethylene-based polymer (B) of the present invention is imparted to an ethylene-based polymer (B).

[0310] In the foregoing pages, three catalyst systems, that is, a catalyst system containing, as an essential component, a complex having a bridged (cyclopentadienyl)(indenyl) ligand or the like, a catalyst system containing, as an essential component, a complex having a benzindenyl ligand or the like, and a catalyst system using a mixture of a complex having a bridged bis(indenyl) ligand or a bridged bis(cyclopentadienyl) ligand, which is a metallocene complex, and a borane or borate compound that is a compound capable of producing a cationic metallocene compound together with an organoaluminum oxy compound, are described as specific preferred examples of the olefin polymerization catalyst for producing a long-chain branched structure suitable as the ethylene-based polymer (B) of the present invention. Among these, a catalyst system containing, as an essential component, a complex having a bridge (cyclopentadienyl)(indenyl) ligand or the like and a catalyst system using a mixture of a complex having a bridged bis(indenyl) ligand or a bridged bis(cyclopentadienyl) ligand, which is a metallocene complex, and a borane or borate compound that is a compound capable of producing a cationic metallocene compound together with an organoaluminum oxy compound, are more preferred, and a catalyst system containing, as an essential component, a complex having a bridged (cyclopentadienyl)(indenyl) ligand or the like is still more preferred.

[0311] In the present invention, the production of the ethylene-based polymer (B) is performed by contacting ethylene with the olefin polymerization catalyst (i) to (iv), more preferably (i), (ii) or (iv), still more preferably (i) or (ii), yet still more preferably (ii) the metallocene catalyst, thereby polymerizing or copolymerizing the ethylene. As the olefin polymerization catalyst, a plurality of kinds of catalyst may be selected from (i) to (iv) and used. At the time of performing polymerization or copolymerization of ethylene, all descriptions of the polymerization method, ethylene raw material, polymerization medium, polymerization temperature and the like, polymerization process and the like, and scavenger in the paragraph of Production Method of Ethylene-Based Polymer (A) above may be referred to. However, it is needless to say that these various conditions must be optimally set by taking into account various characteristics required of the ethylene-based polymer (B) and the characteristics of the olefin polymerization catalyst used. For example, in the case of desiring for an ethylene-based polymer (B) having a lower MFR and a lower density, the chain transfer agent concentration is set relatively low, the α-olefin concentration is set relatively high, in order to prevent a polymer in the production process from a trouble such as fixing•blocking, various operation temperatures are set on the low temperature side as appropriate for the melting temperature or the like of the polymer, a low-molecular-weight hydrocarbon solvent hardly causing dissolution of the polymer such as propane and butane, is selected in the slurry polymerization, a gas phase polymerization not using a solvent is selected, or solution polymerization treating the polymer in the molten state is selected. Also, in the case of intending to impart distinctive long-chain branch characteristics, it is preferred to aggressively select a low monomer concentration condition, a high polymer concentration condition, a low scavenger concentration condition, a high temperature polymerization condition, a long time polymerization condition or the like so that the chain transfer reaction except for hydrogen can be accelerated.

[0312] In the polyethylene-based resin composition of the present invention, as long as the purpose of the present invention is not impaired, the following substances can be blended as an optional component, in addition to the ethylene-based polymer (A) and the ethylene-based polymer (B), which are essential components.

3-1. Other Ethylene-Based Polymers

[0313] In addition to the ethylene-based polymer (A) and the ethylene-based polymer (B), various ethylene-based polymers and modification products thereof, such as high-density polyethylene, low-density polyethylene, high-pressure polyethylene, polar monomer graft-modified polyethylene, ethylene-based wax, ultrahigh molecular weight polyethylene and ethylene-based elastomer, can be used. Addition of a high-density polyethylene is preferred for enhancing the stiffness, heat resistance, impact strength and the like. Addition of a low-density polyethylene is preferred for enhancing the flexibility, impact strength, easy adhesiveness, transparency, low-temperature strength and the like. Addition of a high-pressure polyethylene is preferred for enhancing the flexibility, easy adhesiveness, transparency, low-temperature strength, moldability and the like. Addition of a polar monomer graft-modified polyethylene such as maleic acid-modified polyethylene, ethylene.acrylic acid derivative copolymer and ethylene-vinyl acetate copolymer is preferred for enhancing the flexibility, easy adhesiveness, colorability, affinity for various materials, gas barrier property and the like. Addition of an ethylene-based wax is preferred for enhancing the colorability, affinity for various materials, moldability and the like. Addition of an ultrahigh molecular weight polyethylene is preferred for enhancing the mechanical strength, abrasion resistance and the like. Addition of an ethylene-based elastomer is preferred for enhancing the flexibility, mechanical strength, impact strength and the like.

3-2. Other Olefin-Based Polymer

[0314] As an olefin-based polymer other than an ethylene-based polymer, for example, a polypropylene-based resin, a higher olefin-based resin such as polybutene, polyisobutene and polyhexene, an olefin-based rubber, a polybutadiene-based resin such as butadiene, isoprene and chloroprene, a polystyrene-based resin such as polystyrene and poly-α-methylstyrene, various cyclic olefin-based resin, and modification products thereof can be used.

3-3. Other Resins

[0315] Various resins containing, as a main component, a polymer except for the above-described ethylene-based polymer or other olefin-based polymers can be used. Specific examples thereof include various nylon resins, various polyamides, polyethylene terephthalate (PET), polybutylene terephthalate (PBT), various polyesters, a polycarbonate resin, EVOH, EVA, PMMA, PMA, various engineering plastics, polylactic acid, celluloses, natural rubbers, polyurethane, vinyl chloride, fluororesin such as Teflon (registered trademark), and an inorganic polymer such as silicon resin.

3-4. Additive

[0316] All additives may be appropriately used individually or in combination of two or more thereof. Specifically, for example, an antioxidant (e.g., phenol type, phosphorus type, sulfur type), an ultraviolet absorber•ultraviolet inhibitor, a light stabilizer-weatherproofing agent, a lubricant, an antistatic agent, an antifogging agent, an antiblocking agent, a processing aid such as dispersant, a color pigment (organic or inorganic pigment), a pearl pigment, a polarizing pearl pigment, a crosslinking agent, a blowing agent, a neutralizer, a heat stabilizer, a crystallization nucleating agent, an inorganic or organic bulking agent•filler [such as calcium carbonate, talc, metal powder (e.g., aluminum, copper, iron, lead), silica dust, diatomaceous earth, alumina, gypsum, mica, clay, asbestos, graphite, carbon black and titanium oxide], and a flame retardant can be used.

[0317] The polyethylene-based resin composition of the present invention is produced by mixing the ethylene-based polymer (A), the ethylene-based polymer (B), which are essential components, and the substance (C) as an optional component.

[0318] The blending ratio of respective components is from 41 to 99 wt % of the ethylene-based polymer (A) and from 1 to 59 wt % of the ethylene-based polymer (B), preferably from 61 to 96 wt % of the ethylene-based polymer (A) and from 4 to 39 wt % of the ethylene-based polymer (B), more preferably from 69 to 96 wt % of the ethylene-based polymer (A) and from 4 to 31 wt % of the ethylene-based polymer (B), still more preferably from 69 to 91 wt % of the ethylene-based polymer (A) and from 9 to 31 wt % of the ethylene-based polymer (B), yet still more preferably from 75 to 89 wt % of the ethylene-based polymer (A) and from 11 to 25 wt % of the ethylene-based polymer (B). If the proportion of the ethylene-based polymer (A) is too large, the polyethylene-based resin composition or its molded product may be reduced in the impact resistance or transparency and out of the moldability, the melt tension decreases, whereas if the proportion is small, the stiffness may be deteriorated and out of the moldability, the melt extrudability becomes bad. If the proportion of the ethylene-based polymer (B) is too large, the polyethylene-based resin composition or its molded product may be reduced in the stiffness or transparency and out of the moldability, the melt extrudability becomes bad, whereas if the proportion is small, the tear strength, impact strength and transparency may not be improved and out of the moldability, the melt tension decreases. Incidentally, the proportion of the substance (C) as an optional component is appropriately set as long as the purpose of the present invention is not impaired, but the proportion is usually from 0 to 49 wt % and particularly, in using various additives recited in Item 3-4 above, all existing examples related to application to known polyethylene-based resins, polyethylene-based resin compositions and their molded product may be referred to.

[0319] In producing the polyethylene-based resin composition of the present invention by mixing the ethylene-based polymer (A), the ethylene-based polymer (B), which are essential components, and the substance (C) as an optional component, the mixing method therefor or the apparatus used is not particularly limited, but usually, these components are mixed using a Henschel mixer, a super-mixer, a tumbler-type mixer or the like, kneaded under heating, for example, in a mixing extruder such as single- or twin-screw extruder, kneader and plunger extruder, or in a Banbury mixer, and then pelletized. The kneading under heating can be performed in the presence or absence of a liquid, a solvent or a gas. The order of mixing those components is also not particularly limited, and, for example, the following methods (D-1) to (D-4) may be recited:

[0320] (D-1) a method where the ethylene-based polymer (A), the ethylene-based polymer (B) and the optional substance (C) all in the solid state, preferably all in the powder, particle or pellet state, are previously contacted and mixed with each other, and the mixture is put into a more uniform state by kneading under heating;

[0321] (D-2) a method where any one or more components of the ethylene-based polymer (A), the ethylene-based polymer (B) and the optional substance (C) are put into a molten state, a dissolved state or a liquid state and then contacted and mixed with other components, and the mixture is furthermore put into a more uniform state by kneading under heating;

[0322] (D-3) a method where any two components of the ethylene-based polymer (A), the ethylene-based polymer (B) and the optional substance (C) are previously kneaded under heating by, for example, the method (D-1) or (D-2) above, and the mixture obtained by the kneading under heating is further kneaded under heating with the remaining one component and thereby put into a more uniform state; and

[0323] (D-4) a method where any one component of the ethylene-based polymer (A), the ethylene-based polymer (B) and the optional substance (C) is previously kneaded under heating with, individually and separately, both of the remaining two components, for example, by the method (D-1) or (D-2), and the mixtures obtained by the kneading under heating is further kneaded under heating and thereby put into a more uniform state.

[0324] The polyethylene-based resin composition of the present invention is produced by mixing the ethylene-based polymer (A), the ethylene-based polymer (B), which are essential components, and the substance (C) as an optional component, for example, by the mixing method of (D-1) to (D-4) above, and as for the physical properties, the composition as a whole must satisfy the ranges of MFR and density described below.

5-1. MFR

[0325] The melt flow rate (MFR) of the polyethylene-based resin composition of the present invention is from 0.05 to 50 g/10 min, preferably from 0.1 to 20 g/10 min, more preferably from 0.3 to 10 g/10 min, still more preferably from 0.4 to 5.0 g/10 min, yet still more preferably from 0.5 to 3.0 g/10 min. If MFR is less than 0.05 g/10 min, the flowability of the polyethylene-based resin composition is bad, and this may disadvantageously require a too high motor load of the extruder or lead to poor spreadability. If MFR exceeds 50 g/10 min, the polyethylene-based resin composition or its molded product becomes inferior in the mechanical strength such as impact strength, tear strength and tensile strength or in the moldability, and this is not preferred. Incidentally, MFR indicates a value when measured under the same conditions as the condition (A-1) above.

5-2. Density

[0326] The density of the polyethylene resin composition of the present invention is from 0.910 to 0.960 g/cm³, preferably from 0.910 to 0.950 g/cm³, more preferably from 0.916 to 0.940 g/cm³, still more preferably from 0.919 to 0.938 g/cm³, yet still more preferably from 0.920 to 0.936 g/cm³, and most preferably from 0.921 to 0.934 g/cm³.

[0327] If the density of the polyethylene resin composition is less than 0.910 g/cm³, the polyethylene-based resin composition or its molded product may be reduced in the stiffness or become sticky and when the product is a molded product having a small thickness, such as film and sheet, as well as various problems in using the product, a problem is disadvantageously brought about in the step of winding up the product or the post-processing step such as surface printing•lamination, leading to poor suitability for automatic bag machine, or when the product is a molded product having a large wall thickness, such as pipe and various containers, since the product is too soft and undergoes deformation, the wall thickness must be disadvantageously designed to be larger than necessary. Also, if the density of the polyethylene resin composition exceeds 0.960 g/cm³, the impact strength of the polyethylene-based resin composition or its molded product may be reduced and the transparency may also become bad. Incidentally, the density indicates a value when measured under the same conditions as the condition (A-2) above.

[II] Molded Product and Use of Polyethylene-Based Resin Composition of the Present Invention

[0328] The molded product of the polyethylene-based resin composition of the present invention is produced by molding the polyethylene-based resin composition of the present invention described in [I] above, and as for the molding method, all of molding methods for a polyolefin-based resin or a polyolefin-based resin composition, such as injection molding, compression-injection molding, rotational molding, extrusion molding, hollow molding and blow molding, which are conventionally known, may be referred to.

[0329] The molded product as used in the present invention indicates a processed article or a shaped article obtained by processing or shaping the polyethylene-based resin composition into an appropriate form according to the intended use, and specific examples thereof include a film, a bag, a sheet, a coating, a fiber, a yarn, a container, a tube, a pipe, a covering material, a lid, a cap, a box, sundry articles, toys, medical device parts, a bead, a fine particle, and a foamed product. These articles may have a multilayer structure or may be a composite article with other members. As for these molded articles of the polyethylene-based resin composition of the present invention, specific examples of use thereof include a standardized bag mandated by the dimensional standard, such as bag-in-paper bag and garbage bag, a heavy duty sack, a wrapping film, a sugar bag, a rice bag, an oily substance packaging bag, a food packaging film in a bag for packaging a watery material such as pickles, an agricultural film, a laminate with various substrates such as nylon, polyester, metal foil and saponified ethylene-vinyl acetate copolymer, a foamed body, and a molded product thereof, and applications of a molded product of known polyethylene-based resins and polyethylene-based resin compositions, such as bag-in-box, detergent container, edible oil container, retort container, medical container, chemical container, solvent container, agricultural container, various plastic bottle products, hollow container (e.g., kerosene can, drum, fuel tank), infusion bag, various tubes, pipe (e.g., water pipe, gas pipe), Tupperware container cover, bottle cap and container, may be referred to.

[0330] The molding method for the molded product of the present invention is not particularly limited as long as it is a method capable of effectively utilizing excellent molding characteristics, various mechanical properties and transparency of the polyethylene-based resin composition of the present invention, but in the case of a film, bag or sheet as an example of the application in which the polyethylene-based resin composition of the present invention is intended to be mainly used, preferred examples of the molding method, molding conditions and use include, specifically, various inflation molding methods, T-die film molding methods, calender molding methods, multilayer film molding methods using a multilayer coextrusion molding machine or lamination processing, and various applications, which are described in detail, for example, in JP-A-2007-197722, JP-A-2007-177168, JP-A-2007-177187 and JP-A-2010-31270. Of course, a gas other than air, or a liquid can be used as a cooling medium in the inflation molding and may be also used in special inflation such as stretch (inflation simultaneous biaxial stretching) molding and multi-stage blow-molding.

[0331] The thus-obtained film (or sheet) product is not particularly limited in its sheet, and the suitable thickness differs depending on the molding method•conditions. For example, in the case of inflation molding, the thickness is approximately from 5 to 300 μm, and in the case of T-die molding, a film (or sheet) having a thickness of approximately from 5 μm to 5 mm can be obtained. Similarly, in the case of hollow containers as an example of the application in which the polyethylene-based resin composition of the present invention is intended to be mainly used, preferred examples of the molding method, molding conditions and used include, specifically, various hollow molding methods and blow molding methods and various applications, which are described in detail, for example, in JP-A-2004-18812, JP-A-2009-143079 and JP-A-2009-173889. Similarly, in the case of a pipe, a covering material, a cover, caps, a box and sundries as an example of the application of the polyethylene-based resin composition of the present invention, preferred examples of the molding method, molding conditions and used include, specifically, various molding methods and various applications, which are described in detail, for example, in JP-A-2007-2235, JP-A-2007-177183 and JP-A-2002-60559. Furthermore, as other applications, the polyethylene-based resin composition may be used as a modifier, for example, to enhance the moldability, enhance the mechanical strength, impart low-temperature resistance or impart low-temperature adhesiveness, by blending a small amount of the composition with another polyethylene-based resin or polyethylene-based resin composition or with a polyolefin-based resin such as polypropylene-based resin.

[III] Ethylene-Based Polymer

[0332] A second aspect of the present invention relates to an ethylene-based polymer having a developed long-chain branched structure and exhibiting excellent moldability. The second aspect of the present invention is described below item by item.

[0333] The ethylene-based polymer of the present invention satisfies all of the conditions (B-1′) to (B-8) described below.

III-1. Condition (B-1′)

[0334] MFR_B of the ethylene-based polymer in the present invention is from 0.001 to 200 g/10 min, preferably from 0.01 to 100 g/10 min, more preferably from 0.05 to 50 g/10 min, still more preferably from 0.1 to 50 g/10 min, and most preferably from 0.1 to 10 g/10 min. If MFR_B is less than 0.001 g/10 min, the ethylene-based polymer may be inferior in the moldability, particularly in the melt flowability and spreadability, and uniform mixing with another resin may become difficult, disadvantageously giving rise to production of an appearance failure such as gel, grain and fisheye or reduction in the impact strength or transparency. If MFR_B exceeds 200 g/10 min, the ethylene-based polymer or a composition obtained by mixing the polymer with another resin may be reduced in the mechanical strength such as impact strength, tear strength and tensile strength and this is not preferred. Incidentally, MFR indicates a value when measured under the same conditions as in the condition (A-1).

III-2. Condition (B-2″)

[0335] The density_B of the ethylene-based polymer in the present invention is from 0.880 to 0.970 g/cm³, preferably from 0.891 to 0.960 g/cm³, more preferably from 0.895 to 0.950 g/cm³, still more preferably from 0.900 to 0.934 g/cm³, and most preferably from 0.900 to 0.925 g/cm³. When the density_B is in this range, the ethylene-based polymer or its molded product is excellent in the balance between impact strength and stiffness and in the transparency. On the other hand, if the density_B is less than 0.880 g/cm³, the stiffness is reduced and when the product is a molded product having a small thickness, such as film and sheet, as well as various problems in using the product, a problem is disadvantageously brought about in the step of winding up the product or the post-processing step such as surface printing•lamination or when the product is a molded product having a large wall thickness, such as pipe and various containers, since the product is too soft and undergoes deformation, the wall thickness must be disadvantageously designed to be larger than necessary. In addition, the polymer is heavily sticky even at room temperature and difficult to handle in the blending step with another resin, disadvantageously giving rise to product sticking of the resin composition, and furthermore, the compatibility with the another resin may be reduced to deteriorate the impact strength or transparency due to phase separation. Also, if the density_B exceeds 0.970 g/cm³, the impact strength or transparency is deteriorated and this is not preferred. In the case of using the polymer as a modifier to enhance the strength of another resin, the density of the ethylene-based polymer in the present invention is preferably from 0.900 to 0.910 g/cm³. Incidentally, the density indicates a value when measured under the same conditions as the condition (A-2) above.

III-3. Condition (B-3)

[0336] The [Mw/Mn]_B of the ethylene-based polymer in the present invention is from 2.0 to 10.0, preferably from 2.0 to 6.0, more preferably from 2.5 to 5.6, still more preferably from 2.9 to 4.5, yet still more preferably from 3.2 to 4.0. If [Mw/Mn]_B is less than 2.0, the polymer may be reduced in the molding characteristics or may be difficult to mix with another resin and therefore, this should be avoided. If [Mw/Mn]_B exceeds 10.0, the ethylene-based polymer, the mixed resin composition with another resin or the molded product may lack the impact strength, be deteriorated in the transparency or become sticky, and this is not preferred. Incidentally, Mw/Mn indicates a value measured under the same conditions as the condition (A-3) above.

III-4. Condition (B-4′)

[0337] The [λmax(2.0)]_B of the ethylene-based polymer in the present invention is from 1.2 to 30.0, preferably from 1.5 to 20.0, more preferably from 2.0 to 10.0, still more preferably from 2.4 to 6.0, yet still more preferably from 3.0 to 5.0. If [λmax(2.0)]_B is less than 1.2, the ethylene-based polymer, the mixed resin composition with another resin or the molded product may lack the flowability or melt tension and be deteriorated in the molding characteristics. If [λmax(2.0)]_B exceeds 30.0, the flowability and melt tension may be excellent, but the ethylene-based polymer or the like may be disadvantageously reduced in the impact strength or transparency. Incidentally, hλmax(2.0) indicates a value when measured under the same conditions as the condition (A-4) above. The effect of the elongational flow characteristics of the polyethylene on its moldability or mechanical properties of the molded product is as already described above in the condition (A-4) or condition (B-4).

III-5. Condition (B-5)

[0338] As regards the ethylene-based polymer in the present invention, the [λmax(2.0)]_B/[λmax(0.1)]_B defined in the condition (B-5) of Item 2.5 above is from 1.2 to 10.0, preferably from 1.3 to 5.0, more preferably from 1.4 to 4.0, still more preferably from 1.5 to 3.0. If [λmax(2.0)]_B/[λmax(0.1)]_B is less than 1.2, the ethylene-based polymer, the mixed resin composition with another resin or the molded product may be in a non-uniform molten state or may have a thermally unstable structure, or reduction in the impact strength or deterioration of the transparency may be caused due to strength anisotropy of the molded product, which is attributable to the presence of a significantly elongated long-chain branched structure, and this is not preferred. If [λmax(2.0)]_B/[λmax(0.1)]_B exceeds 10.0, the melt tension and flowability during molding may be excellent, but the ethylene-based polymer, the mixed resin composition with another resin or the molded product may be disadvantageously reduced in the impact strength or transparency.

III-6. Condition (B-6)

[0339] The ethylene-based polymer of the present invention is a polymer produced by an ethylene polymerization reaction using a catalyst containing a transition metal, and all of the matters described in the condition (B-6) of Item 2.6 apply.

III-7. Condition (B-7)

[0340] As regards the ethylene-based polymer in the present invention, the above-described g_C′ is from 0.30 to 0.70, and all of the matters described in the condition (B-7) of Item 2.7 above apply. The g_C′ value is preferably from 0.30 to 0.59, more preferably from 0.35 to 0.55, still more preferably from 0.35 to 0.50, yet still more preferably from 0.35 to 0.45. If the g_C′ value exceeds 0.70, the ethylene-based polymer, the mixed resin composition with another resin or the molded product may disadvantageously lack the moldability or transparency. If the g_C′ value is less than 0.30, the moldability of the ethylene-based polymer or the like may be improved, but the impact strength of the molded product may be reduced or the transparency may be deteriorated, and this is not preferred. Incidentally, the g_C′ value or the W_C value in the next paragraph indicates a value when measured under the same conditions as the condition (B-7) of Item 2.7 or the condition (B-8) of Item 2.8 above.

III-8. Condition (B-8)

[0341] As regards the ethylene-based polymer in the present invention, the above-described W_C is from 0.01 to 30.0%, and all of the matters described in the condition (B-8) of Item 2.8 above apply. The W_C value is more preferably from 0.02 to 10.0%, still more preferably from 0.05 to 8.0%, yet still more preferably from 0.10 to 6.0%, and most preferably from 0.11 to 4.0%. If the W_C value is less than 0.01%, the ethylene-based polymer or the mixed resin composition with another resin may be inferior in the moldability or the ethylene-based polymer or the like may lack the transparency, and this is not preferred. If the W_C value exceeds 30.0%, the ethylene-based polymer or the like may be enhanced in the melt tension out of the moldability, but the melt flowability may be excessively reduced to disadvantageously cause a problem in the production or molding of the ethylene-based polymer or the like. Furthermore, the impact strength or the transparency of the molded product may be deteriorated, and this is not preferred.

III-9. Condition (B-9)

[0342] The ethylene-based polymer in the present invention preferably further satisfies the following condition (B-9), in addition to the condition (B-1′) to the condition (B-8) defined in Items III-1 to III-8 above.

[0343] The condition (B-9) is that in the TREF measurement using an orthodichlorobenzene solvent, the content (W₋₁₅; unit: wt %) of components eluted at −15° C. is 2.0 wt % or less.

[0344] The W₋₁₅ value is preferably 0.9 wt % or less, more preferably 0.6 wt % or less, still more preferably 0.5 wt %, yet still more preferably 0.4 wt %, and most preferably 0.3 wt %. The lower limit of the W₋₁₅ value is preferably 0.0 wt %, that is, the components are not detected. If the W₋₁₅ value exceeds 2.0 wt %, the ethylene-based polymer, the mixed resin composition with another resin or the molded product may lack the impact strength, be deteriorated in the transparency or become sticky, and this is not preferred. Also, the compatibility with another resin may become bad, and this may disadvantageously give rise to deterioration of the impact strength or transparency. In the present invention, the W₁₅ value is measured by the following method.

[0345] A sample is dissolved in orthodichlorobenzene (containing 0.5 mg/mL BHT) at 140° C. to prepare a solution, and the solution is introduced into a TREF column at 140° C., then cooled to 100° C. at a temperature drop rate of 8° C./min, further cooled to −15° C. at a temperature drop rate of 4° C./min and held for 60 minutes. Thereafter, orthodichlorobenzene (containing 0.5 mg/mL BHT) as a solvent is flowed through the column at a flow rate of 1 mL/min to elute components dissolved in the orthodichlorobenzene at −15° C. in the TREF column for 10 minutes, and then the column temperature is raised linearly to 140° C. at a temperature rise rate of 100° C./hr to obtain an elution curve.

Apparatus:

[0346] TREF Column: Stainless steel-made column of 4.3 mmφ×150 mm

[0347] Column packing material: Inert glass bead of 100 μm

[0348] Heating system: Aluminum heating block

[0349] Cooling system: Peltier element (cooling of Peltier element is water cooling)

[0350] Temperature distribution: +0.5° C.

[0351] Temperature regulator: programmable digital controller, KP 1000, manufactured by Chino Corporation

[0352] Heating system: Air bath oven

[0353] Temperature at measurement: 140° C.

[0354] Temperature distribution: 1° C.

[0355] Valve: Six-way valve, four-way valve

[0356] Injection system: Loop injection system

[0357] Injection amount: Loop size, 0.1 ml

[0358] Injection port heating system: Aluminum heating block

[0359] Temperature at measurement: 140° C.

[0360] Detector: Wavelength-fixed infrared detector, MIRAN 1A, manufactured by FOXBORO

[0361] Detection wavelength: 3.42 μm

[0362] High-temperature flow cell: Micro-flowcell for LC-IR, optical path length: 1.5 mm, window shape: oval of 2×4 mm, synthetic sapphire aperture plate

[0363] Temperature at measurement: 140° C.

[0364] Liquid delivery pump: SSC-3461 pump, manufactured by Senshu Kagaku Measurement Conditions:

[0365] Solvent: o-Dichlorobenzene (containing 0.5 mg/mL of BHT)

[0366] Sample concentration: 5 mg/mL

[0367] Sample injection amount: 0.1 mL

[0368] Solvent flow velocity: 1 mL/min

[IV] Olefin Polymerization Catalyst Component of the Present Invention

[0369] A third aspect of the present invention relates to an olefin polymerization catalyst component containing a metallocene compound having a specific structure, which is useful for producing a metallocene-based polyolefin or metallocene-based polyethylene having a sufficient number of long-chain branches having an appropriate length, and an olefin polymerization catalyst containing the component. The third aspect of the present invention is described below item by item.

[0370] The olefin polymerization catalyst component of the present invention is an olefin polymerization catalyst component containing the following component (A-1b) and component (A-2b), or an olefin polymerization catalyst component containing the following component (Ac).

IV-1. Olefin Polymerization Catalyst Component Containing Component (A-1b) and Component (A-2b) of the Present Invention

[0371] A first embodiment of the olefin polymerization catalyst component of the present invention contains the components (A-1b) and (A-2b) defined below as essential components.

[0372] Component (A-1b): a metallocene compound represented by the following formula (1b):

[0373]
[in formula (1b), M^1b represents any one transition metal of Ti, Zr and Hf; each of X^1b and X^2b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; each of Q^1b and Q^2b independently represents a carbon atom, a silicon atom or a germanium atom; each R^1b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and at least two members out of four R^1b may combine to form a ring together with Q^1b and Q^2b; m^b is 0 or 1 and when m^b is 0, Q^1b is bonded directly to the conjugated 5-membered ring including R^2b and R^3b; and each of R^2b, R^3b and R^4b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40 and out of R^2b, R^3b and R^4b, only either one pair of adjacent R^3b and R^3b and adjacent R^2b and R^3b may form a ring together with the carbon atoms to which the pair is bonded].

[0374] Component (A-2b): a metallocene compound represented by the following formula (2b):

[0375]
[in formula (2b), M^2b represents any one transition metal of Ti, Zr and Hf; each of X^11b and X^12b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; Q^11b represents a carbon atom, a silicon atom or a germanium atom; each R^11b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and two R^11b may combine with each other to form a ring together with Q^11b; each of R^12b, R^14b and R^15b independently represents an atom or a group selected from a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, and a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, provided that at least one member is not a hydrogen atom; each R^13b independently represents a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40; and out of R^12b, R^13b, R^14b and R^15b, any only one pair of adjacent R^12b and R^12b, adjacent R^13b and R^13b and adjacent R^12b and R^13b and any only one pair of adjacent R^14b and R^14b, adjacent R^15b and R^15b and adjacent R^14b and R^15b may form a ring together with the carbon atoms to which the pair is bonded].

[0376] The components (A-1b) and (A-2b) (hereinafter, both are sometimes collectively referred to as component (Ab) or simply as Ab) are specifically described below.

IV-[(1). Component (A-1b)

[0377] The olefin polymerization catalyst component of the present invention is characterized by containing a metallocene compound represented by formula (1b) as the component (A-1b).

[0378] In formula (1b), M^1b of the metallocene compound represents Ti, Zr or Hf, preferably represents Zr or Hf, more preferably represents Zr.

[0379] Each of X^1b and X^2b specifically includes, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a methoxymethyl group, an ethoxymethyl group, an n-propoxymethyl group, an i-propoxymethyl group, an n-butoxymethyl group, an i-butoxymethyl group, a tert-butoxymethyl group, a methoxyethyl group, an ethoxyethyl group, an acetyl group, a 1-oxopropyl group, a 1-oxo-n-butyl group, a 2-methyl-1-oxopropyl group, a 2,2-dimethyl-1-oxo-propyl group, a phenylacetyl group, a diphenylacetyl group, a benzoyl group, a 2-methoxyphenyl group, a 3-methoxyphenyl group, a 4-methoxyphenyl group, a 2-furyl group, a 2-tetrahydrofuryl group, a dimethylaminomethyl group, a diethylaminomethyl group, a di-i-propylaminomethyl group, a bis(dimethylamino)methyl group, a bis(di-i-propylamino)methyl group, a (dimethylamino)(phenyl)methyl group, a methylimino group, an ethylimino group, a 1-(methylimino)ethyl group, a 1-(phenylimino)ethyl group, a 1-[(phenylmethyl)imino]ethyl group, an ethoxy group, an n-propoxy group, an i-propoxy group, an n-butoxy group, an i-butoxy group, a tert-butoxy group, a phenoxy group, a dimethylamino group, a diethylamino group, a di-n-propylamino group, a di-i-propylamino group, a di-n-butylamino group, a di-i-butylamino group, a di-tert-butylamino group, and a diphenylamino group.

[0380] Specific preferred examples of X^1b and X^2b include a chlorine atom, a bromine atom, a methyl group, an n-butyl group, an i-butyl group, a methoxy group, an ethoxy group, an i-propoxy group, an n-butoxy group, a phenoxy group, a dimethylamino group, and a di-i-propylamino group. Among these specific examples, a chlorine atom, a methyl group and a dimethylamino group are more preferred.

[0381] Each of Q^b and Q^2b independently represents a carbon atom, a silicon atom or a germanium atom and is preferably a carbon atom or a silicon atom.

[0382] Each R^1b independently includes, for example, a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, and a phenyl group. In the case where at least two R^1b are combined to form a ring together with Q^1b and Q^2b, examples include a cyclobutylidene group, a cyclopentylidene group, a cyclohexylidene group, a silacyclobutyl group, a silacyclopentyl group, and a silacyclohexyl group.

[0383] When Q^1b or/and Q^2b are a carbon atom, specific preferred examples of R^1b include a hydrogen atom, a methyl group, an ethyl group, a phenyl group and a cyclobutylidene group, and when Q^1b or/and Q^2b are a silicon atom, specific preferred examples include a methyl group, an ethyl group, a phenyl group and a silacyclobutyl group.

[0384] Each of R^2b, R^3b and R^4b specifically includes, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, and a 2-(trimethyl)silylfuryl group.

[0385] Out of R^2b, R^3b and R^4b, any one or more members are preferably a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20, because the polymerization activity is particularly increased.

[0386] Specific preferred examples of R^2b, R^3b and R^4b include a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a 2-methylfuryl group, and a trimethylsilyl group. Among these specific examples, a hydrogen atom, a methyl group, an n-butyl group, a tert-butyl group, a phenyl group and a trimethylsilyl group are more preferred, and a hydrogen atom, a methyl group, a tert-butyl group and a phenyl group are still more preferred.

[0387] Specific examples of the condensed cyclopentadienyl structure formed by adjacent two R^3b and a cyclopentadienyl moiety to which both R^3b are bonded, include the following partial structures (I) to (VI), and specific examples of the condensed cyclopentadienyl structure formed by adjacent R^3b and R^2b and a cyclopentadienyl moiety to which these R^3b and R^2b are bonded, are the same.

[0388] Among these specific examples, (I), (III) and (VI) are preferred. Also, R^4b may be substituted on these partial structures (I) to (VI).

[0389]

[0390] In formula (1b), m^b is 0 or 1 and when m^b is 0, Q^1b is bonded directly to the conjugated 5-membered ring including R^2b and R^3b.

[0391] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-1b) is preferably a compound represented by the following formula (3b):

[0392]
[in formula (3b), M^1b represents any one transition metal of Ti, Zr and Hf; each of X^1b and X^2b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; each of Q^1b and Q^2b independently represents a carbon atom, a silicon atom or a germanium atom; each R^1b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and at least two members out of four R^1b may combine to form a ring together with Q^1b and Q^2b; m^b is 0 or 1 and when m^b is 0, Q^1b is bonded directly to the conjugated 5-membered ring including R^2b and R^3b; and each of R^2b, R^3b and R^4b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40 and out of R^2b, R^3b and R^4b, only either one pair of adjacent R^3b and R^3b and adjacent R^2b and R^3b may form a ring together with the carbon atoms to which the pair is bonded].

[0393] In formula (3b), detailed definitions of M^1b, X^1b, X^2b, Q^1b, Q^2b, R^1b, R^2b, R^3b and R^4b follow the definitions in the description of formula (1b) above.

[0394] In formula (3b), particularly when R^3b is a hydrogen atom, R^2b is preferably a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 6 and while one of two R^4b is a hydrogen atom, the remaining one is preferably a hydrogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, specifically, the remaining one R^4b is preferably a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a 2-(trimethyl)silylfuryl group or the like; and R^2b is more preferably a hydrogen atom and while one of two R⁴ is a hydrogen atom, the remaining one is more preferably a hydrogen atom, a hydrocarbon group having a carbon number of 1 to 20, or a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, specifically, the remaining one R^4b is more preferably a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group or the like. The remaining one R^4b is specifically, still more preferably a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group or a triphenylsilyl group, and the remaining one R^4b is specifically, yet still more preferably a hydrogen atom, an n-butyl group, an i-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group or a triphenylsilyl group.

[0395] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-1b) is more preferably a compound represented by the following formula (4b):

[0396]
[in formula (4b), M^1b represents any one transition metal of Ti, Zr and Hf; each of X^1b and X^2b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; each of Q^1b and Q^2b independently represents a carbon atom, a silicon atom or a germanium atom; each R^1b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and at least two members out of four R^1b may combine to form a ring together with Q^1b and Q^2b; m^b is 0 or 1 and when m^b is 0, Q^1b is bonded directly to the conjugated 5-membered ring including R^2b, R^5b and R^6b; and each of R^2b and R^4b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40 and R^4b does not form a ring together with the carbon atom to which R^4b is bonded; R^5b represents a saturated or unsaturated divalent hydrocarbon group having a carbon number of 4 or 5 for forming a condensed ring with the 5-membered ring to which R^5b is bonded; R^6b is an atom or a group bonded to a carbon atom of R^5b and each independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom and having a carbon number of 1 to 20, or a hydrocarbon group-substituted silyl group having a carbon number of 1 to 20; and n^b represents an integer of 0 to 10 and when n^b is 2 or more, at least two R^6b may form a ring together with the carbon atoms to which R^6b are bonded].

[0397] In formula (4b), detailed definitions of M^1b, X^1b, X^2b, Q^1b, Q^2b, R^1b, R^2b and R^4b follow the definitions in the description of formula (1b) above. Specific examples of the condensed cyclopentadienyl structure formed by R^5b and a cyclopentadienyl moiety to which R^5b is bonded, include the partial structures (I) to (VI). Among these specific examples, (I), (III) and (VI) are preferred. Also, R^6b may be substituted on these partial structures (I) to (VI).

[0398] The substituent R^6b includes, in addition to a hydrogen atom, for example, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 4-tert-butylphenyl group, a 3,5-dimethylphenyl group, a 3,5-di-tert-butylphenyl group, a naphthyl group, an anthracenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 2,6-dichloro-4-trimethylsilylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, and a 2-(trimethyl)silylfuryl group. R^6b may form a ring together with the carbon atom to which R^6b is bonded. Also, in formula (4b), particularly when R^2b is a hydrogen atom, all of two R^4b and R^6b are preferably a hydrogen atom or at least any one of two R^4b and R^6b is preferably a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, specifically, at least any one is preferably a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a 2-(trimethyl)silylfuryl group or the like. In another preferred embodiment when R^2b in formula (4b) is a hydrogen atom, while either one of two R^4b is a hydrogen atom, the remaining one is preferably a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, specifically, the remaining one R^4b is preferably a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a 2-(trimethyl)silylfuryl group or the like; and while either one of two R^4b is a hydrogen atom, the remaining one is more preferably a hydrocarbon group having a carbon number of 1 to 20 or a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, specifically, the remaining one R^4b is preferably a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group or the like. The remaining one R^4b is specifically, still more preferably a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group or a triphenylsilyl group; and the remaining one R^4b is specifically, yet still more preferably an n-butyl group, an i-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group or a triphenylsilyl group. Furthermore, in formula (4b), particularly when R^4b is a hydrogen atom, each of R^2b and R^6b is preferably any one of a hydrogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, and a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, specifically, each of R^2b and R^6b is preferably any one of a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, a 2-(trimethyl)silylfuryl group and the like; and each of R^2b and R^6b is more preferably a hydrogen atom, a hydrocarbon group having a carbon number of 1 to 20, or a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, specifically, each of R^2b and R^6b is more preferably a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group or the like. Each of R^2b and R^6b is specifically, still more preferably a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group, or a triphenylsilyl group, and each of R^2b and R^6b is specifically, yet still more preferably a hydrogen atom, an n-butyl group, an i-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group or a triphenylsilyl group.

[0399] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-1b) is still more preferably a compound represented by the following formula (5b):

[0400]
[in formula (5b), M^1b represents any one transition metal of Ti, Zr and Hf; each of X^1b and X^2b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; Q^1b represents a carbon atom, a silicon atom or a germanium atom; each R^1b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and two R^1b may combine with each other to form a ring together with Q^1b; and each of R^2b, R^4b and R^6b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40 and R^4b does not form a ring together with the carbon atom to which R^4b is bonded; and R^6b may form a ring together with the carbon atoms to which R^6b is bonded].

[0401] In formula (5b), detailed definitions of M^1b, X^b, X^2b, Q^1b, R^1b, R^2b, R^4b and R^6b follow the definitions in the description of formula (4b) above. The substituent R^6b is preferably a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 4-tert-butylphenyl group, a 3,5-dimethylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group or a 2-(trimethyl)silylfuryl group, more preferably a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group or a phenyl group, still more preferably a hydrogen atom, a methyl group, an n-butyl group, a tert-butyl group, a phenyl group or a trimethylsilyl group, yet still more preferably a hydrogen atom, a methyl group, a tert-butyl group or a phenyl group. In the case where the substituents R^6b form a ring together with the carbon atom to which the substituents are bonded, preferably, adjacent two R^6b form a 6-membered ring structure together with the carbon atoms to which these substituents are bonded; more preferably, both R^6b on the 4-position and the 5-position combine to form a 6-membered ring structure; and still more preferably, a benzindenyl ring structure is formed as a whole together with the indenyl ring to which the substituents are bonded.

[0402] In the olefin polymerization catalyst component of the present invention, specific examples of the metallocene compound as the component (A-1b) of the olefin polymerization catalyst component are illustrated below, but the present invention is not limited thereto. Incidentally, the number indicating the position of each substituent on the cyclopentadienyl ring, indenyl ring and azulenyl ring of metallocene compounds recited as specific examples of the component (A-1b) and the later-described (A-2b) is as shown in the following formulae.

[0403]

[0404] (i) The metallocene compounds classified into a bridged Cp(Ind)Zr type include, for example, those shown in Table b-1 below.

[0405]

TABLE b-1
(i) Bridged Cp(Ind)Zr Type
		No.	A1	A2	A3
		1b	dimethylsilylene	Cl	Cl
		2b	dimethylsilylene	Me	Me
		3b	dimethylsilylene	Ph	Ph
		4b	isopropylidene	Cl	Cl
		5b	silacyclobutyl	Cl	Cl
		6b	silacyclopentyl	Cl	Cl
		7b	silacyclohexyl	Cl	Cl
		8b	cyclobutylidene	Cl	Cl
		9b	cyclopentylidene	Cl	Cl
		10b	cyclohexylidene	Cl	Cl
		11b	dimethylgermirene	Cl	Cl

[0406] (ii) The metallocene compounds classified into a bridged Cp(3-substituted Ind)Zr type include, for example, those shown in Tables b-2 and b-3 below.

[0407]

TABLE b-2
(ii) Bridged Cp(3-Substituted Ind)Zr Type
No.	A1	A2	A3	A4	A5
12b	dimethylsilylene	3-methyl	—	chloride	chloride	C
13b	dimethylsilylene	3-methyl	—	methyl	methyl	C
14b	isopropylidene	3-methyl	—	chloride	chloride	A
15b	dimethylsilylene	3-ethyl	—	chloride	chloride	B
16b	isopropylidene	3-ethyl	—	chloride	chloride	A
17b	dimethylsilylene	3-n-propyl	—	chloride	chloride	B
18b	isopropylidene	3-n-propyl	—	chloride	chloride	A
19b	dimethylsilylene	3-i-propyl	—	chloride	chloride	B
20b	isopropylidene	3-i-propyl	—	chloride	chloride	A
21b	dimethylsilylene	3-n-butyl	—	chloride	chloride
22b	isopropylidene	3-n-butyl	—	chloride	chloride
23b	dimethylsilylene	3-tert-butyl	—	chloride	chloride
24b	cyclobutylidene	3-tert-butyl	—	chloride	chloride
25b	dimethylsilylene	3-tert-butyl	—	methyl	methyl
26b	isopropylidene	3-tert-butyl	—	chloride	chloride
27b	dimethylsilylene	3-n-pentyl	—	chloride	chloride
28b	dimethylsilylene	3-n-hexyl	—	chloride	chloride
29b	dimethylsilylene	3-cyclohexyl	—	chloride	chloride	B
30b	dimethylsilylene	3-phenyl	—	chloride	chloride
31b	dimethylsilylene	3-benzyl	—	chloride	chloride	B
32b	dimethylsilylene	3-tolyl	—	chloride	chloride
33b	dimethylsilylene	3-trimethylsilyl	—	chloride	chloride	A
34b	dimethylsilylene	3-chlorophenyl	—	chloride	chloride	A
35b	dimethylsilylene	3-fluorophenyl	—	chloride	chloride	B
36b	dimethylsilylene	3-(5-methyl-2-furyl)	—	chloride	chloride	C
37b	dimethylsilylene	—	4-methyl	chloride	chloride	B
38b	dimethylsilylene	—	5-methyl	chloride	chloride	B
39b	dimethylsilylene	—	6-methyl	chloride	chloride	C
40b	dimethylsilylene	3-methyl	4-methyl	chloride	chloride
41b	dimethylsilylene	3-tert-butyl	4-methyl	chloride	chloride	C
42b	dimethylsilylene	—	4-phenyl	chloride	chloride	C
43b	dimethylsilylene	—	4-(4-methylphenyl)	chloride	chloride	C
44b	dimethylsilylene	—	4-(4-tert-butylphenyl)	chloride	chloride
45b	dimethylgermirene	3-methyl	—	chloride	chloride

[0408]

TABLE b-3
(ii) Bridged Cp(3-substituted Ind)Zr Type (continued)
No.	A1	A2	A3	A4	A5
46b	dimethylgermirene	3-ethyl	—	chloride	chloride
47b	dimethylgermirene	3-i-propyl	—	chloride	chloride
48b	dimethylgermirene	3-n-butyl	—	chloride	chloride
49b	dimethylgermirene	3-tert-butyl	—	chloride	chloride
50b	diethylsilylene	—	—	chloride	chloride	C
51b	diethylsilylene	3-methyl	—	chloride	chloride	B
52b	diethylsilylene	3-ethyl	—	chloride	chloride	B
53b	diethylsilylene	3-i-propyl	—	chloride	chloride
54b	diethylsilylene	3-n-butyl	—	chloride	chloride
55b	diethylsilylene	3-tert-butyl	—	chloride	chloride
56b	di-n-butylsilylene	—	—	chloride	chloride	C
57b	di-n-butylsilylene	3-methyl	—	chloride	chloride	B
58b	di-n-butylsilylene	3-ethyl	—	chloride	chloride	B
59b	di-n-butylsilylene	3-i-propyl	—	chloride	chloride
60b	di-n-butylsilylene	3-n-butyl	—	chloride	chloride
61b	di-n-butylsilylene	3-tert-butyl	—	chloride	chloride
62b	diphenylsilylene	—	—	chloride	chloride
63b	diphenylmethylene	—	—	chloride	chloride	C
64b	diphenylsilylene	3-methyl	—	chloride	chloride	B
65b	diphenylsilylene	3-ethyl	—	chloride	chloride	B
66b	diphenylsilylene	3-i-propyl	—	chloride	chloride
67b	diphenylsilylene	3-n-butyl	—	chloride	chloride
68b	diphenylsilylene	3-tert-butyl	—	chloride	chloride	C
69b	dimethylsilylene	—	benz[e]	chloride	chloride	C
70b	dimethylsilylene	—	dibenzo	chloride	chloride
71b	dimethylsilylene	—	azulenyl	chloride	chloride	C
72b	dimethylsilylene	—	4-methylazulenyl	chloride	chloride	C
73b	dimethylsilylene	—	4-phenylazulenyl	chloride	chloride	B
74b	dimethylsilylene	—	5,6-dimethyl	chloride	chloride	C
75b	dimethylsilylene	—	benz[f]	chloride	chloride
76b	dimethylsilylene	—	6,7-dihydroindacenyl	chloride	chloride
77b	dimethylsilylene	—	5,5,7,7-tetramethyl-6,7-	chloride	chloride
			dihydroindacenyl
78b	dimethylsilylene	—	5,6,7,8-tetra-	chloride	chloride
			hydrobenz[f]
79b	dimethylsilylene	—	5,6,7,8-tetrahydro-5,5,8,8-	chloride	chloride
			tetramethylbenz[f]

[0409] (iii) The metallocene compounds classified into a bridged (3-substituted Cp)(Ind)Zr type include, for example, those shown in Table b-4 below.

[0410]

TABLE b-4
(iii) Bridged (3-Substituted Cp)(Ind)Zr Type
No.	A1	A2	A3	A4	A5
80b	dimethylsilylene	4-methyl	—	chloride	chloride	C
81b	dimethylsilylene	4-ethyl	—	chloride	chloride	C
82b	dimethylsilylene	4-i-propyl	—	chloride	chloride	C
83b	dimethylsilylene	4-n-butyl	—	chloride	chloride	C
84b	dimethylsilylene	4-i-butyl	—	chloride	chloride	C
85b	dimethylsilylene	4-tert-butyl	—	chloride	chloride	C
86b	dimethylsilylene	4-tert-butyl	—	bromide	bromide	C
87b	dimethylsilylene	4-tert-butyl	—	methyl	methyl	C
88b	dimethylsilylene	4-tert-butyl	—	phenyl	phenyl	C
89b	dimethylsilylene	4-tert-butyl	4,5,6,7-	chloride	chloride	C
			tetrahydro
90b	dimethylsilylene	4-tert-butyl	azulenyl	chloride	chloride	C
91b	dimethylsilylene	4-	—	chloride	chloride	C
		trimethylsilyl
92b	dimethylsilylene	4-(2-	—	chloride	chloride	A
		bromoethyl)
93b	dimethylsilylene	4-(2-	—	chloride	chloride	C
		trimethyl-
		silylfuryl)
94b	dimethylsilylene	4-phenyl	—	chloride	chloride	C
95b	dimethylsilylene	4-(4-	—	chloride	chloride	C
		methylphenyl)
96b	isopropylidene	4-tert-butyl	—	chloride	chloride	A
97b	dimethylgermirene	4-tert-butyl	—	chloride	chloride

[0411] (iv) The metallocene compounds classified into a bridged (4-substituted Cp)(3-substituted Ind)Zr type include, for example, those shown in Table b-5 below.

[0412]

TABLE b-5
(iv) Bridged (4-Substituted Cp)(3-Substituted Ind)Zr Type
No.	A1	A2	A3	A4	A5	A6
98b	dimethylsilylene	4-tert-	3-	—	chloride	chloride
		butyl	methyl
99b	dimethylsilylene	4-tert-	3-tert-	—	chloride	chloride
		butyl	butyl
100b	dimethylsilylene	4-tert-	3-tert-	—	chloride	chloride
		butyl	butyl
101b	dimethylsilylene	4-tert-	—	4-	chloride	chloride
		butyl		phenyl
102b	dimethylsilylene	3,4-	3-tert-	—	chloride	chloride
		dimethyl	butyl
103b	isopropylidene	4-tert-	3-n-	—	chloride	chloride
		butyl	butyl
104b	dimethylsilylene	4-tert-	—	4-	chloride	chloride
		butyl		phenyl-
				azulenyl

[0413] (v) The metallocene compounds classified into a bridged bisCpZr type include, for example, those shown in Table b-6 below.

[0414]

TABLE b-6
(v) Bridged bisCpZr Type
	No.	A1	A2	A3
	105b	dimethylsilylene	chloride	chloride
	106b	dimethylsilylene	methyl	methyl
	107b	dimethylsilylene	phenyl	phenyl
	108b	dimethylsilylene	benzyl	benzyl
	109b	isopropylidene	chloride	chloride
	110b	silacyclobutyl	chloride	chloride
	111b	dimethylgermirene	chloride	chloride

[0415] (vi) The metallocene compounds classified into a bridged Cp(3-substituted Cp)Zr type include, for example, those shown in Table b-7 below.

[0416]

TABLE b-7
(vi) Bridged Cp(3-substituted Cp)Zr Type
No.	A1	A2	A3	A4
112b	dimethylsilylene	3-n-propyl	chloride	chloride	C
113b	dimethylsilylene	3-tert-butyl	chloride	chloride	C
114b	dimethylsilylene	3-cyclohexyl	chloride	chloride	C
115b	dimethylsilylene	3-biphenyl	chloride	chloride	C
116b	dimethylsilylene	3-(4-methylphenyl)	chloride	chloride	C
117b	dimethylsilylene	3-(5-methyl-2-furyl)	chloride	chloride	C
118b	dimethylsilylene	3-tert-butyl-4-methyl	chloride	chloride	B
119b	dimethylsilylene	3-tert-butyl-4-ethyl	chloride	chloride	B
120b	isopropylidene	3-tert-butyl	chloride	chloride	A
121b	dimethylgermirene	3-tert-butyl	chloride	chloride

[0417] (vii) The metallocene compounds classified into a bridged bis(3-substituted Cp)Zr type include, for example, those shown in Table b-8 below.

[0418]

TABLE b-8
(vii) Bridged bis (3-substituted Cp)Zr Type
No.	A1	A2	A3	A4	A5
122b	dimethylsilylene	3-tert-butyl	3-tert-butyl	chloride	chloride
123b	dimethylsilylene	3-tert-butyl	3-tert-butyl	methyl	methyl
124b	dimethylsilylene	3-tert-butyl	3-tert-butyl	phenyl	phenyl
125b	isopropylidene	3-tert-butyl	3-tert-butyl	chloride	chloride
126b	silacyclobutyl	3-tert-butyl	3-tert-butyl	chloride	chloride
127b	dimethyl-	3-tert-butyl	3-tert-butyl	chloride	chloride
	germirene
128b	dimethylsilylene	3-allyl	3-allyl	chloride	chloride
129b	dimethylsilylene	3-	3-	chloride	chloride
		trimethylsilyl	trimethylsilyl
130b	dimethylsilylene	3-ethyl-	3-ethyl-	chloride	chloride
		4-methyl	4-methyl
131b	dimethylsilylene	3-tert-butyl-	3-tert-butyl-	chloride	chloride
		4-methyl	4-methyl
132b	dimethylsilylene	3-(2-	3-(2-	chloride	chloride
		bromoethyl)	bromoethyl)
133b	dimethylsilylene	3-(4-	3-(4-	chloride	chloride
		chlorophenyl)	chlorophenyl)
134b	dimethylsilylene	3-benzyl	3-benzyl	chloride	chloride
135b	dimethylsilylene	3-(5-methyl-	3-(5-methyl-	chloride	chloride
		2-furyl)	2-furyl)
136b	dimethylsilylene	3-tert-butyl	3-methyl	chloride	chloride
137b	dimethylsilylene	3-tert-butyl	4-tert-butyl	chloride	chloride
138b	dimethylsilylene	3-methyl	4-phenyl	chloride	chloride
139b	dimethylsilylene	3,4-dimethyl	3-tert-butyl	chloride	chloride
140b	dimethylsilylene	3,4-dimethyl	3-(2-	chloride	chloride
			methylfuryl)
141b	dimethylsilylene	3-methyl-4-	3-tert-butyl-	chloride	chloride
		phenyl	4-ethyl

[0419] The metallocene compound also includes, for example, compounds where zirconium of the compounds above is replaced by titanium or hafnium.

[0420] Furthermore, in using these metallocene compounds as the component (A-1b), two or more thereof may be also used.

[0421] In specific compounds exemplified above, in terms of excellent performance in both polymerization activity and moldability, preferred metallocene compounds as the component (A-1b) are denoted by “A”, more preferred compounds are denoted by “B”, and still more preferred compounds are denoted by “C”.

[0422] Synthesis examples for the metallocene compound as the component (A-1b) according to the present invention are described below, but the present invention is not limited to these synthesis methods in particular.

[0423] For example, there are a method where an indene compound is lithiated, then reacted with a dichlorosilane compound and subsequently reacted with cyclopentadienyl lithium to obtain a ligand and the obtained ligand is reacted with a tetrakis(alkylamido)zirconium and then with trimethylsilyl chloride, and a method where the obtained ligand is lithiated and subsequently reacted with zirconium tetrachloride.

IV-[(2). Component (A-2b)

[0424] The olefin polymerization catalyst component of the present invention is characterized by containing a metallocene compound represented by formula (2b) as the component (A-2b).

[0425] In formula (2b), M^2b of the metallocene compound represents Ti, Zr or Hf, preferably represents Zr or Hf, more preferably represents Zr.

[0426] Each of X^11b and X^12b specifically includes, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a methoxymethyl group, an ethoxymethyl group, an n-propoxymethyl group, an i-propoxymethyl group, an n-butoxymethyl group, an i-butoxymethyl group, a tert-butoxymethyl group, a methoxyethyl group, an ethoxyethyl group, an acetyl group, a 1-oxopropyl group, a 1-oxo-n-butyl group, a 2-methyl-1-oxopropyl group, a 2,2-dimethyl-1-oxo-propyl group, a phenylacetyl group, a diphenylacetyl group, a benzoyl group, a 2-methoxyphenyl group, a 3-methoxyphenyl group, a 4-methoxyphenyl group, a 2-furyl group, a 2-tetrahydrofuryl group, a dimethylaminomethyl group, a diethylaminomethyl group, a di-i-propylaminomethyl group, a bis(dimethylamino)methyl group, a bis(di-i-propylamino)methyl group, a (dimethylamino)(phenyl)methyl group, a methylimino group, an ethylimino group, a 1-(methylimino)ethyl group, a 1-(phenylimino)ethyl group, a 1-[(phenylmethyl)imino]ethyl group, an ethoxy group, an n-propoxy group, an i-propoxy group, an n-butoxy group, an i-butoxy group, a tert-butoxy group, a phenoxy group, a dimethylamino group, a diethylamino group, a di-n-propylamino group, a di-i-propylamino group, a di-n-butylamino group, a di-i-butylamino group, a di-tert-butylamino group, and a diphenylamino group.

[0427] Specific preferred examples of X^11b and X^12b, each independently, include a chlorine atom, a bromine atom, a methyl group, an n-butyl group, an i-butyl group, a methoxy group, an ethoxy group, an i-propoxy group, an n-butoxy group, a phenoxy group, a dimethylamino group, and a di-i-propylamino group. Among these specific examples, a chlorine atom, a methyl group and a dimethylamino group are more preferred.

[0428] Q^11b represents a carbon atom, a silicon atom or a germanium atom and is preferably a carbon atom or a silicon atom.

[0429] Each R^11b independently includes, for example, a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, and a phenyl group. In the case where R^11b forms a ring together with Q^1b, examples include a cyclobutylidene group, a cyclopentylidene group, a cyclohexylidene group, a silacyclobutyl group, a silacyclopentyl group, and a silacyclohexyl group.

[0430] When Q^11b is a carbon atom, specific preferred examples of R^11b include a hydrogen atom, a methyl group, an ethyl group, a phenyl group and a cyclobutylidene group, and when Q^11b is a silicon atom, specific preferred examples include a methyl group, an ethyl group, a phenyl group and a silacyclobutyl group.

[0431] Each of R^12b, R^14b and R^15b specifically includes an element or a group selected from, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, and a 2-(trimethyl)silylfuryl group, provided that at least one member thereof is not a hydrogen atom; specifically, each is preferably an element or a group selected from a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a trimethylsilyl group, a furyl group, a 2-methylfuryl group and a 2-(trimethyl)silyl group, provided that at least one member thereof is not a hydrogen atom; and specifically, each is more preferably an element or a group selected from a hydrogen atom, a methyl group, an n-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group, provided that at least one member thereof is not a hydrogen atom. The member that is not a hydrogen atom is preferably at least one member out of R^12b located on the 2-position of the cyclopentadienyl ring, R^14b located on the same 2-position and two R^15b; the member that is not a hydrogen atom is more preferably at least one member out of R^12b located on the 2-position of the cyclopentadienyl ring and two R^15b; and the member that is not a hydrogen atom is still more preferably at least one member out of R^12b located on the 2-position of the cyclopentadienyl ring and R^15b located on the same 2-position.

[0432] Each R^13b independently includes, for example, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, and a 2-(trimethyl)silylfuryl group; preferably, each is independently a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a trimethylsilyl group, a furyl group, a 2-methylfuryl group or a 2-(trimethyl)silyl group; and more preferably, each is independently an element or a group selected from a methyl group, an n-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group.

[0433] In formula (2b), adjacent R^12b and R^12b may form a condensed cyclopentadienyl structure of the partial structure (I) to (VI) described in the component (A-1b), preferably a condensed cyclopentadienyl structure of (I), (III) or (VI), together with the carbon atom on the cyclopentadienyl ring, to which those members are bonded, but in this case, the ring structure above is not formed between adjacent R^13b and R^13b and between adjacent R^12b and R^13b. Similarly, adjacent R^13b and R^13b may form a condensed cyclopentadienyl structure of (I) to (VI), preferably a condensed cyclopentadienyl structure of (I), (III) or (VI), but in this case, the ring structure above is not formed between adjacent R^2b and R^12b and between adjacent R^12b and R^13b. Also, similarly, adjacent R^12b and R^13b may form a condensed cyclopentadienyl structure of (I) to (VI), preferably a condensed cyclopentadienyl structure of (I), (III) or (VI), but in this case, the ring structure above is not formed between adjacent R^12b and R^12b and between adjacent R^13b and R^13b

[0434] Furthermore, in formula (2b), adjacent R^14b and R^14b may form a condensed cyclopentadienyl structure of (I) to (VI), preferably a condensed cyclopentadienyl structure of (I), (III) or (VI), but in this case, the ring structure above is not formed between adjacent R^15b and R^15b and between adjacent R^14b and R^15b. Similarly, adjacent R^15b and R^15b may form a condensed cyclopentadienyl structure of (I) to (VI), preferably a condensed cyclopentadienyl structure of (I), (III) or (VI), but in this case, the ring structure above is not formed between adjacent R^14b and R^14b and between adjacent R^14b and R^15b. Also, similarly, adjacent R^14b and R^15b may form a condensed cyclopentadienyl structure of (I) to (VI), preferably a condensed cyclopentadienyl structure of (I), (III) or (VI), but in this case, the ring structure above is not formed between adjacent R^14b and R^14b and between adjacent R^15b and R^15b

[0435] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-2b) is preferably a compound represented by the following formula (6b):

[0436]
[in formula (6b), M^2b represents any one transition metal of Ti, Zr and Hf; each of X^11b and X^12b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; Q^11b represents a carbon atom, a silicon atom or a germanium atom; each R^11b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and two R^11b may combine with each other to form a ring together with Q^11b each of R^12b and R^14b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, provided that R^12b and R^14b do not form a ring together with the carbon atoms to which these members are bonded; each of R^16b and R^17b independently represents a saturated or unsaturated divalent hydrocarbon group having a carbon number of 4 or 5 for forming a condensed ring with the 5-membered ring to which R^16b or R^17b is bonded; each of R^18b and R^19b is an atom or a group bonded to a carbon atom of R^16b or R^17b and each independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40; each of p^b and q^b independently represents an integer of 0 to 10 and when each of p^b and q^b is 2 or more, at least two R^18b or at least two R^19b may form a ring together with the carbon atoms to which these members are bonded].

[0437] In formula (6b), detailed definitions of M^2b, X^11b, X^12b, Q^11b and R^11b follow the definitions in the description of formula (2b) above.

[0438] In formula (6b), each of R^12b and R^14b specifically includes an element or a group selected from, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, and a 2-(trimethyl)silylfuryl group; specifically, each is preferably an element or a group selected from a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a trimethylsilyl group, a furyl group, a 2-methylfuryl group and a 2-(trimethyl)silyl group; and specifically, each is more preferably an element or a group selected from a hydrogen atom, a methyl group, an n-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group. Also, at least one member out of R^12b located on the 2-position of the cyclopentadienyl ring and R^14b located on the same 2-position is more preferably a group selected from a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a trimethylsilyl group, a furyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group, still more preferably a group selected from a methyl group, an n-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group.

[0439] Specific examples of the condensed cyclopentadienyl structure formed by R^16b and a cyclopentadienyl moiety to which R^16b is bonded, include the partial structures (I) to (VI). Among these specific examples, (I), (III) and (VI) are preferred. Also, R^18b may be substituted on these partial structures (I) to (VI).

[0440] The substituent R^18b includes, in addition to a hydrogen atom, for example, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 4-tert-butylphenyl group, a 3,5-dimethylphenyl group, a 3,5-di-tert-butylphenyl group, a naphthyl group, an anthracenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 2,6-dichloro-4-trimethylsilylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, and a 2-(trimethyl)silylfuryl group. R^8b may form a ring together with the carbon atom to which R^18b is bonded.

[0441] In formula (6b), each of R^17b and R^19b is also independently defined, similarly to R^16b and R^18b.

[0442] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-2b) is also preferably a compound represented by the following formula (7b):

[0443]
[in formula (7b), M^2b represents any one transition metal of Ti, Zr and Hf; each of X^11b and X^12b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; Q^11b represents a carbon atom, a silicon atom or a germanium atom; each R^11b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and two R^11b may combine with each other to form a ring together with Q^11b; each of R^12b, R^14b and R^15b independently represents an atom or a group selected from a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, and a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, provided that at least one of R^12b, R^14b and R^15b located on the 2-position and 5-position of both cyclopentadienyl rings is not a hydrogen atom and R^12b, R^14b and R^15b do not form a ring together with the carbon atoms to which these members are bonded; R^16b represents a saturated or unsaturated divalent hydrocarbon group having a carbon number of 4 or 5 for forming a condensed ring with the 5-membered ring to which R^16b is bonded; R^18b is an atom or a group bonded to a carbon atom of R^16b and each independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40; p^b represents an integer of 0 to 10 and when p^b is 2 or more, at least two R^18b may form a ring together with the carbon atoms to which these members are bonded].

[0444] In formula (7b), detailed definitions of M^2b, X^11b, X^12b, Q^11b, R^11b, R^16b and R^18b follow the definitions in the description of formula (6b) above.

[0445] In formula (7b), each of R^12b, R^14b and R^15b specifically includes an element or a group selected from, for example, a hydrogen atom, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, a phenyldimethylsilyl group, a furyl group, a tetrahydrofuryl group, a 2-methylfuryl group, and a 2-(trimethyl)silylfuryl group, provided that at least one of R^12b, R^14b and R^15b located on the 2-position and 5-position of both cyclopentadienyl rings is not a hydrogen atom; specifically, each is preferably an element or a group selected from a hydrogen atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a trimethylsilyl group, a furyl group, a 2-methylfuryl group and a 2-(trimethyl)silyl group, provided that at least one of R^12b, R^14b and R^15b located on the 2-position and 5-position of both cyclopentadienyl rings is not a hydrogen atom; and specifically, each is more preferably an element or a group selected from a hydrogen atom, a methyl group, an n-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group, provided that at least one of R^12b, R^14b and R^15b located on the 2-position and 5-position of both cyclopentadienyl rings is not a hydrogen atom. In formula (7b), R^12b located on the 2-position of the cyclopentadienyl ring is more preferably an atom or a group selected from a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, and a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40; still more preferably a group selected from a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a trimethylsilyl group, a furyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group; and most preferably a group selected from a methyl group, an n-butyl group, a tert-butyl group, a phenyl group, a trimethylsilyl group, a 2-methylfuryl group and a 2-(trimethyl)silylfuryl group. In formula (7b), R^12b, R^14b and R^15b do not form a ring together with the carbon atoms to which these members are bonded.

[0446] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-2b) is more preferably a compound represented by the following formula (8b):

[0447]
[in formula (8b), M^2b represents any one transition metal of Ti, Zr and Hf; each of X^1b and X^12b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; Q^11b represents a carbon atom, a silicon atom or a germanium atom; each R^11b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and two R^1b may combine with each other to form a ring together with Q^11b; each of R^12b, R^14b, R^18b and R^19b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, provided that R^12b and R^14b do not form a ring together with the carbon atoms to which these members are bonded; and R^18b and R^19b may form a ring together with the carbon atoms to which these members are bonded].

[0448] In formula (8b), detailed definitions of M^2b, X^11b, X^12b, Q^11b, R^11b, R^12b, R^14b, R^18b and R^19b follow the definitions in the description of formula (6b) above.

[0449] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-2b) is also more preferably a compound represented by the following formula (9b):

[0450]
[in formula (9b), M^2b represents any one transition metal of Ti, Zr and Hf; each of X^11b and X^12b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a nitrogen atom and having a carbon number of 1 to 20, a hydrocarbon group-substituted amino group having a carbon number of 1 to 20, or an alkoxy group having a carbon number of 1 to 20; Q^11b represents a carbon atom, a silicon atom or a germanium atom; each R^11b independently represents a hydrogen atom or a hydrocarbon group having a carbon number of 1 to 10 and two R^11b may combine with each other to form a ring together with Q^11b; each of R^12b, R^14b and R^15b independently represents a hydrogen atom, a halogen atom, a hydrocarbon group having a carbon number of 1 to 20, a silicon-containing hydrocarbon group containing from 1 to 6 silicons and having a carbon number of 1 to 18, a halogen-containing hydrocarbon group having a carbon number of 1 to 20, a hydrocarbon group containing an oxygen atom or a sulfur atom and having a carbon number of 1 to 40, or a silyl group substituted with a hydrocarbon group having a carbon number of 1 to 40, provided that at least one of R^12b located on the 2-position of the indenyl ring and R^14b and R^15b located on the 2-position and 5-position of the cyclopentadienyl ring is not a hydrogen atom and R^12b, R^14b and R^15b do not form a ring together with the carbon atoms to which these members are bonded; and R^18b may form a ring together with the carbon atom to which R^18b is bonded].

[0451] In formula (9b), detailed definitions of M^2b, X^11b, X^12b, Q^11b, R^11b, R^12b, R^14b, R^15b and R^18b follow the definitions in the description of formula (6b) above.

[0452] As the olefin polymerization catalyst component according to the present invention, the metallocene compound of the component (A-2b) is, out of the compounds represented by formulae (2b) and (6b) to (9b), preferably a compound where R^12b as a substituent on the 2-position of the conjugated 5-membered ring is a halogen atom, an alkyl group having a carbon number of 1 to 6, an alkoxy group having a carbon number of 1 to 6, a phenoxy group having a carbon number of 6 to 12, an alkenyl group having a carbon number of 2 to 8, a halogen-containing alkyl group having a carbon number of 1 to 6, an aryl group having a carbon number of 6 to 18, a halogen-containing aryl group having a carbon number of 6 to 18, an alkyl group having a carbon number of 1 to 3 and containing a trialkylsilyl group with the alkyl group having a carbon number of 1 to 3, a silyl group containing a hydrocarbon group having a carbon number of 1 to 6, an oxygen-containing heterocyclic group or a sulfur-containing heterocyclic group. Such a preferred substituent R^12b on the 2-position specifically includes, for example, a chlorine atom, a bromine atom, an iodine atom, a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, a neopentyl group, a cyclopentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group, a benzyl group, a 2-methylphenyl group, a 3-methylphenyl group, a 4-methylphenyl group, a 3,5-dimethylphenyl group, a 4-tert-butylphenyl group, a 3,5-di-tert-butylphenyl group, a bis(trimethylsilyl)methyl group, a bis(tert-butyldimethylsilyl)methyl group, a bromomethyl group, a chloromethyl group, a 2-chloroethyl group, a 2-bromoethyl group, a 2-bromopropyl group, a 3-bromopropyl group, a 2-bromocyclopentyl group, a 2,3-dibromocyclopentyl group, a 2-bromo-3-iodocyclopentyl group, a 2,3-dibromocyclohexyl group, a 2-chloro-3-iodocyclohexyl group, a 2-chlorophenyl group, a 4-chlorophenyl group, a 2,3,4,5,6-pentafluorophenyl group, a 4-trifluoromethylphenyl group, a trimethylsilyl group, a tri-tert-butylsilyl group, a di-tert-butylmethylsilyl group, a tert-butyldimethylsilyl group, a triphenylsilyl group, a diphenylmethylsilyl group, and a phenyldimethylsilyl group; specifically, is more preferably a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclohexyl group, a phenyl group or a trimethylsilyl group; and specifically, is still more preferably a methyl group, an n-butyl group, a tert-butyl group, a phenyl group or a trimethylsilyl group.

[0453] Other specific examples of the chemical structure for the preferred substituent R^12b on the 2-position include an oxygen-containing heterocyclic group and a sulfur-containing heterocyclic group, represented by the following formula (10b):

[0454]

[0455] In formula (10b), R^21b and R^22b may be the same as or different from each other and is a hydrogen atom, a halogen atom, an alkyl group having a carbon number of 1 to 6, an alkoxy group having a carbon number of 1 to 6, an alkenyl group having a carbon number of 2 to 8, a halogen-containing alkyl group having a carbon number of 1 to 6, an aryl group having a carbon number of 6 to 18, a halogen-containing aryl group having a carbon number of 6 to 18, an alkyl group having a carbon number of 1 to 3 and containing a trialkylsilyl group with the alkyl group having a carbon number of 1 to 3, or a silyl group containing a hydrocarbon group having a carbon number of 1 to 6. Both of R^21b and R^22b may together constitute a 6- or 7-membered ring, and the 6- or 7-membered ring may contain an unsaturated bond.

[0456] Here, specific examples of the alkyl group having a carbon number of 1 to 6 include a methyl group, an ethyl group, an n-propyl group, an i-propyl group, an n-butyl group, an i-butyl group, a s-butyl group, a tert-butyl group, an n-pentyl group, an n-hexyl group, a cyclopropyl group, a cyclopentyl group, and a cyclohexyl group.

[0457] Specific examples of the alkoxy group having a carbon number of 1 to 6 include a methoxy group, an ethoxy group, an n-propoxy group, an i-propoxy group, an n-butoxy group, an i-butoxy group, a tert-butoxy group, and a phenoxy group. The halogen atom includes a chlorine atom, a bromine atom, an iodine atom, and a fluorine atom. Specific examples of the alkenyl group having a carbon number of 2 to 8 include a vinyl group, a propenyl group, an allyl group, a butenyl group, and a cyclohexenyl group. Furthermore, the halogen atom in the halogen-containing alkyl group having a carbon number of 1 to 6 includes a fluorine atom, a chlorine atom, a bromine atom, and an iodine atom. The halogen-containing alkyl group having a carbon number of 1 to 6 is a group where a hydrogen atom on the skeleton of an alkyl group having a carbon number of 1 to 6 is substituted for by a halogen atom, and specific examples thereof include fluoromethyl, difluoromethyl, trifluoromethyl chloromethyl, dichloromethyl, trichloromethyl, bromomethyl, dibromomethyl, tribromomethyl, iodomethyl, 2,2,2-trifluoroethyl, 2,2,1,1-tetrafluoroethyl, pentafluoroethyl, pentachloroethyl, pentafluoropropyl, nonafluorobutyl, 5-chloropentyl, 5,5,5-trichloropentyl, 5-fluoropentyl, 5,5,5-trifluoropentyl, 6-chlorohexyl, 6,6,6-trichlorohexyl, 6-fluorohexyl, and 6,6,6-trifluorohexyl. The aryl group having a carbon number of 6 to 18 may be substituted with a hydrocarbon group having a carbon number of 1 to 6, and specific examples include phenyl, tolyl, dimethylphenyl, ethylphenyl, trimethylphenyl, tert-butylphenyl, biphenyl, 1-naphthyl, 2-naphthyl, acenaphthyl, phenanthryl, and anthryl. Specific examples of the halogen-containing aryl group having a carbon number of 6 to 18 are those where a hydrogen atom of the above-described aryl group having a carbon number of 6 to 18 is substituted for by a halogen atom, and specific examples include a 2-, 3- or 4-substituted fluorophenyl, a 2-, 3- or 4-substituted chlorophenyl, a 2-, 3- or 4-substituted bromophenyl, a 2,4-, 2,5-, 2,6- or 3,5-substituted difluorophenyl, a 2,4-, 2,5-, 2,6- or 3,5-substituted dichlorophenyl, a 2,4,6-, 2,3,4-, 2,4,5- or 3,4,5-substituted trifluorophenyl, a 2,4,6-, 2,3,4-, 2,4,5- or 3,4,5-substituted trichlorophenyl, pentafluorophenyl, pentachlorophenyl, 3,5-dimethyl-4-chlorophenyl, and 3,5-dichloro-4-biphenyl. The alkyl group having a carbon number of 1 to 3 and containing a trialkylsilyl group with the alkyl group having a carbon number of 1 to 3 is a group where a hydrogen atom of an alkyl group having a carbon number of 1 to 3 is substituted for by a trialkylsilyl group containing an alkyl group having a carbon number of 1 to 3, which may be different, and specific examples thereof include a trimethylsilylmethyl and a trimethylsilylethyl. The silyl group containing a hydrocarbon group having a carbon number of 1 to 6 is a substituent where three hydrocarbon group having a carbon number of 1 to 6, which may be different, are substituted on silicon. The hydrocarbon having a carbon number of 1 to 6 includes an alkyl group having a carbon number of 1 to 6, alkoxy group having a carbon number of 1 to 6, an alkenyl group having a carbon number of 2 to 8, a halogen-containing alkyl group having a carbon number of 1 to 6, and a phenyl group, which are described above, and a substituent may be substituted on the phenyl group. The silyl group containing a hydrocarbon group specifically includes trimethylsilyl, triethylsilyl, tri-n-butylsilyl, tert-butyldimethylsilyl, trivinylsilyl, triallylsilyl, and triphenylsilyl.

[0458] Each of R^21b and R^22b is independently, preferably hydrogen atom, a halogen atom, an alkyl group having a carbon number of 1 to 6, an aryl group having a carbon number of 6 to 18, or a silyl group containing a hydrocarbon group having a carbon number of 1 to 6. In the case where R^21b is a hydrogen atom, the synthesis yield is low, and R^21b is preferably a substituent except for a hydrogen atom. R^21b is more preferably an alkyl group having a carbon number of 1 to 6, an aryl group having a carbon number of 6 to 18, or a silyl group containing a hydrocarbon group having a carbon number of 1 to 6. R^22b is more preferably a hydrogen atom or an alkyl group having a carbon number of 1 to 6. As for specific preferred substituents, R^21b is a methyl group, an ethyl group, a tert-butyl group, a cyclohexyl group, a phenyl group, a trimethylsilyl group or a triphenylsilyl group, and R^22b is a hydrogen atom, a methyl group or an ethyl group.

[0459] Both of R^21b and R^22b may together constitute a 6- or 7-membered ring, and the 6- or 7-membered ring may contain an unsaturated bond. As for specific substitution, the substituent on the 2-position of the indene ring includes a benzofuryl group and a benzothienyl group.

[0460] In the olefin polymerization catalyst component of the present invention, specific examples of the metallocene compound as the component (A-2b) of the olefin polymerization catalyst component are recited below, but the present invention is not limited thereto.

[0461] (i) Examples include: metallocene compounds classified into the bridged Cp₂Zr type; out of compounds recited in the above-described literatures such as JP-A-2-76887, JP-A-3-12406, JP-A-3-12407, JP-A-3-12407, JP-A-11-315089, JP-A-2009-143901 and JP-T-2005-507961, bridged bis(alkyl-substituted cyclopentadienyl)zirconium compounds belonging to formula (2b); and out of zirconium compounds having a cyclopentadienyl ring substituted, for example, with an oxygen-containing hydrocarbon group, a sulfur-containing hydrocarbon group or a hydrocarbon group-substituted silyl group described in JP-T-2002-535339 and the like and belonging to formula (2b), bridged bis(alkyl-substituted cyclopentadienyl)zirconium compounds belonging to formula (2b).

[0462] Metallocene compounds classified into the bridged Cp₂Zr type are shown in Table b-9 and Table b-10.

[0463]

TABLE b-9
(i) Bridged Cp2Zr Type
No.	A1	A2	A3	A4	A5
142b	Me2Si	2,3-Me2	2-Me	Cl	Cl	A	B	C
143b	Me2Si	2,3-Me2	3-Me	Cl	Cl		B
144b	Me2Si	2,3-Me2	4-Me	Cl	Cl		B
145b	Me2Si	2,3-Me2	5-Me	Cl	Cl		B	C
146b	Me2Si	2,3-Me2	2-Et	Cl	Cl		B	C
147b	Me2Si	2,3-Me2	3-Et	Cl	Cl		B
148b	Me2Si	2,3-Me2	2-iPr	Cl	Cl		B	C
149b	Me2Si	2,3-Me2	3-iPr	Cl	Cl		B
150b	Me2Si	2,3-Me2	2-nBu	Cl	Cl		B	C
151b	Me2Si	2,3-Me2	3-tBu	Cl	Cl		B
152b	Me2Si	2,3-Me2	3-Ph	Cl	Cl		B
153b	Me2Si	2,4,5-Me3	—	Cl	Cl
154b	Me2Si	2-Et-4,5-Me2	—	Cl	Cl
155b	Me2Si	2-Et-4-Bu-5-Me	—	Cl	Cl
156b	Me2Si	2,4,5-Me3	2-Me	Cl	Cl		B	C
157b	Me2Si	2-Et-4,5-Me2	3-tBu	Cl	Cl	A	B
158b	Me2Si	2,3,4,5-Me4	—	Cl	Cl	A
159b	Me2Si	2,3,4,5,-Me4	2-Me	Cl	Cl	A	B	C
160b	Me2Si	2,3-Me2	2,3-Me2	Cl	Cl	A	B	C
161b	Me2Si	2,3,-Me2	2,3,-Me2	Br	Br	A	B	C
162b	Me2Si	2,3-Me2	2,3-Me2	Me	Me	A	B	C
163b	Me2Si	2,3,-Me2	2,3,-Me2	Ph	Ph	A	B	C
164b	Me2Si	2,4,5-Me3	2,4,5-Me3	Cl	Cl	A	B	C
165b	Me2Si	2-Et-4,5-Me2	2-Et-4,5-Me2	Cl	Cl	A	B	C

[0464]

TABLE b-10
(i) Bridged Cp2Zr Type (continued)
No.	A1	A2	A3	A4	A5
166b	Me2Si	2-Et-4-Bu-5-Me	2-Et-4-Bu-5-Me	Cl	Cl	A	B	C
167b	Me2Si	2,3,4-Me3	2,3,4-Me3	Cl	Cl	A	B	C
168b	Me2Si	2-Et-3,5-Me2	2-Et-3,5-Me2	Cl	Cl	A	B	C
169b	Me2Si	2,3,4,5-Me4	2,3,4,5-Me4	Cl	Cl	A	B	C
170b	Me2Si	2,3,5-Me3	2,3,5-Me3	Cl	Cl	A	B	C
171b	Me2Si	TMS	2-Ind	Cl	Cl	A	B
172b	Me2Si	1-Ind	2-Ind	Cl	Cl	A	B
173b	Me2Si	3-(2-furyl)-2,5-dimethyl	3-(2-furyl)-2,5-dimethyl	Cl	Cl	A	B	C
174b	Me2Si	2-(2-furyl)-3,5-dimethyl	2-(2-furyl)-3,5-dimethyl	Cl	Cl	A	B	C
175b	Me2Si	2-(2-furyl)-4,5-dimethyl	2-(2-furyl)-4,5-dimethyl	Cl	Cl	A	B	C
176b	Me2Si	3-(2-thienyl)-2,5-dimethyl	3-(2-thienyl)-2,5-dimethyl	Cl	Cl	A	B	C
177b	Me2Si	2-(2-thienyl)-4,5-dimethyl	2-(2-thienyl)-4,5-dimethyl	Cl	Cl	A	B	C
178b	Me2Si	2-(5-methyl-2-furyl)-4,5-	2-(5-methyl-2-furyl)-4,5-	Cl	Cl	A	B	C
		dimethyl	dimethyl
179b	Me2Si	2-(5-tert-butyl-2-furyl)-4,5-	2-(5-tert-butyl-2-furyl)-4,5-	Cl	Cl	A	B	C
		dimethyl	dimethyl
180b	Me2Si	2-(5-trimethyl-	2-(5-trimethyl-	Cl	Cl	A	B	C
		silyl-2-furyl)-4,5-dimethyl	silyl-2-furyl)-4,5-dimethyl
181b	Me2Si	2-(4,5-dimethyl-2-furyl)-4,5-	2-(4,5-dimethyl-2-furyl)-4,5-	Cl	Cl	A	B	C
		dimethyl	dimethyl
182b	Me2Si	2-(2-benzofuryl)-4,5-dimethyl	2-(2-benzofuryl)-4,5-dimethyl	Cl	Cl	A	B	C
183b	Me2C	2-(2-furyl)-3-methyl	2-(2-furyl)-3-methyl	Cl	Cl	A	B	C
184b	Me2C	2-(2-furyl)-3,5-dimethyl	2-(2-furyl)-3,5-dimethyl	Cl	Cl		B	C
185b	Me2C	2-(2-furyl)-4-ethyl-5-methyl	2-(2-furyl)-4-ethyl-5-methyl	Cl	Cl		B	C
186b	Me2C	2-(2-furyl)-4-isopropyl-5-	2-(2-furyl)-4-isopropyl-5-	Cl	Cl		B	C
		methyl	methyl
187b	Me2C	2-(2-furyl)-4-tert-butyl-5-	2-(2-furyl)-4-tert-butyl-5-	Cl	Cl		B	C
		methyl	methyl
188b	Me2C	2-(2-furyl)-4-phenyl-5-methyl	2-(2-furyl)-4-phenyl-5-methyl	Cl	Cl		B	C

[0465] (ii) Examples include metallocene compounds classified into the bridged Ind₂Zr type; out of compounds recited in the above-described literatures such as JP-A-8-59724, JP-A-10-231314, JP-A-2003-105029 and JP-A-2004-352707, bridged bis(substituted or unsubstituted indenyl)zirconium compounds, bridged bis(substituted or unsubstituted azulenyl)zirconium compounds and bridged (substituted or unsubstituted indenyl)(substituted or unsubstituted azulenyl)zirconium compounds belonging to formula (6b) and formula (8b); and out of compounds recited in the above-described literatures such as JP-T-2002-535339 and JP-A-2004-352707, zirconium compounds having an indenyl or azulenyl ring substituted, for example, with an oxygen-containing hydrocarbon group, a sulfur-containing hydrocarbon group or a hydrocarbon group-substituted silyl group and belonging to formula (6b) and formula (8b).

[0466] Metallocene compounds classified into the bridged Ind₂Zr type are shown in Table b-11 and Table b-12.

[0467]

TABLE b-11
(ii) Bridged Ind2Zr Type
No.	A1	A2	A3	A4
189b	Me2Si	Ind	Ind	Cl	A	B
190b	Me2Si	Ind	Ind	Me	A	B
191b	Me2Si	Ind	Ind	Ph	A	B
192b	Me2C	Ind	Ind	Cl		B
193b	Me2Si	H4Ind	H4Ind	Cl	A	B
194b	PhMeSi	H4Ind	H4Ind	Cl	A	B
195b	Me2Si	2,4,4-Me3—H4Ind	2,4,4-Me3—H4Azu	Cl	A	B	C
196b	Me2Si	2-Me—Ind	2-Me—Ind	Cl	A	B	C
197b	Me2Si	2,4-Me2—Ind	2,4-Me2—Ind	Cl	A	B	C
198b	Me2Si	2-Me-4-Ph—Ind	2-Me-4-Ph—Ind	Cl	A	B	C
199b	Me2Si	2-Me-4,5-BenInd	2-Me-4,5-BenInd	Cl	A	B	C
200b	Me2Si	2,4-Me2—H6Azu	2,4-Me2—H6Azu	Cl	A	B	C
201b	Me2Si	2,4-Me2—H4Ind	2,4-Me2—H4Ind	Cl	A	B	C
202b	Me2C	2-Me-4-(4-BiPh)—Azu	2-Me-4-(4-BiPh)—Azu	Cl		B	C
203b	Me2Si	2-Me-4-Ph—Ind	2,4-Ph2—Ind	Cl	A	B	C
204b	Me2Si	2-Me-4-Ph—Ind	2-iPr-4-Ph	Cl	A	B	C
205b	Me2Si	2-Me-4-(p-tBu—Ph)—Ind	2-iPr-4-(p-tBu—Ph)—Ind	Cl	A	B	C
206b	Me2Si	2-(2-furyl)-indenyl	2-(2-furyl)-indenyl	Cl	A	B	C
207b	Me2Ge	2-(2-furyl)-indenyl	2-(2-furyl)-indenyl	Cl
208b	Me2Si	2-(2-thienyl)-indenyl	2-(2-thienyl)-indenyl	Cl	A	B	C
209b	H2C	(2-(2-furyl)-indenyl	(2-(2-furyl)-indenyl	Cl		B	C
210b	Me2C	2-(2-furyl)-indenyl	2-(2-furyl)-indenyl	Cl		B	C
211b	Me2Si	2-(2-furyl)-4,5,6,7-	2-(2-furyl)-4,5,6,7-	Cl	A	B	C
		tetrahydroindenyl	tetrahydroindenyl
212b	Me2C	2-(2-furyl)-7-methyl-indenyl	2-(2-furyl)-7-methyl-indenyl	Cl		B	C
213b	Me2C	2-(2-furyl)-4-methyl-indenyl	2-(2-furyl)-4-methyl-indenyl	Cl		B	C
214b	Me2C	2-(2-furyl)-3-methyl-indenyl	2-(2-furyl)-3-methyl-indenyl	Cl		B	C
215b	Me2C	2-(2-furyl)-3,7-dimethyl-	2-(2-furyl)-3,7-dimethyl-	Cl		B	C
		indenyl	indenyl
216b	Me2C	2-(2-furyl)-4-chloro-indenyl	2-(2-furyl)-4-chloro-indenyl	Cl		B	C
217b	Me2C	2-(2-furyl)-4-phenyl-indenyl	2-(2-furyl)-4-phenyl-indenyl	Cl	A	B	C

[0468]

TABLE b-12
(ii) Bridged Ind2Zr Type (continued)
No.	A1	A2	A3	A4
218b	Me2C	2-(2-furyl)-4-methoxy-indenyl	2-(2-furyl)-4-methoxy-indenyl	Cl		B	C
219b	Me2C	2-(2-furyl)-4-phenoxy-indenyl	2-(2-furyl)-4-phenoxy-indenyl	Cl		B	C
220b	Me2C	2-(2-furyl)-4-trimethylsilyl-	2-(2-furyl)-4-trimethylsilyl-	Cl		B	C
		indenyl	indenyl
221b	Me2Si	2-(2-furyl)-4-phenyl-indenyl	2-(2-furyl)-4-phenyl-indenyl	Cl		B	C
222b	Me2Si	2-(2-furyl)-4-phenyl-indenyl	2-(2-furyl)-4-phenyl-indenyl	Me	A	B	C
223b	Me2Si	2-(2-thienyl)-4-phenyl-indenyl	2-(2-thienyl)-4-phenyl-indenyl	Cl	A	B	C
224b	Me2Si	2-(3-furyl)-4-phenyl-indenyl	2-(3-furyl)-4-phenyl-indenyl	Cl	A	B	C
225b	Me2Si	2-(3-methyl-2-furyl)-indenyl	2-(3-methyl-2-furyl)-indenyl	Cl	A	B	C
226b	Me2Si	2-(3-methyl-2-furyl))-4-phenyl-	2-(3-methyl-2-furyl))-4-phenyl-	Cl	A	B	C
		indenyl	indenyl
227b	Me2Si	2-(2-furyl)-4-(4-	2-(2-furyl)-4-(4-	Cl	A	B	C
		isopropylphenyl)-indenyl	isopropylphenyl)-indenyl
228b	Me2Si	2-(2-furyl)-4,7-diphenyl-	2-(2-furyl)-4,7-diphenyl-	Cl	A	B	C
		indenyl	indenyl
229b	Me2Si	2-(2-furyl)-4-phenyl-7-methyl-	2-(2-furyl)-4-phenyl-7-methyl-	Cl	A	B	C
		indenyl	indenyl
230b	Me2Si	2-(2-furyl)-4-chloro-indenyl	2-(2-furyl)-4-chloro-indenyl	Cl	A	B	C
231b	Me2Si	2-(2-furyl)-4-phenyl-indenyl	2-(2-furyl)-4-phenyl-indenyl	Cl	A	B	C
232b	Me2Si	2-(2-furyl)-4-methoxy-indenyl	2-(2-furyl)-4-methoxy-indenyl	Cl	A	B	C
233b	Me2Si	2,4-di(2-furyl)-indenyl	2,4-di(2-furyl)-indenyl	Cl	A	B	C
234b	Me2Si	2-(2-furyl)-4-(2-thienyl)-	2-(2-furyl)-4-(2-thienyl)-	Cl	A	B	C
		indenyl	indenyl
235b	Me2Si	2-(2-furyl)-4-(2-benzofuryl)-	2-(2-furyl)-4-(2-benzofuryl)-	Cl	A	B	C
		indenyl	indenyl
236b	Me2Si	2-(2-furyl)-benzoindenyl	2-(2-furyl)-benzoindenyl	Cl	A	B	C
237b	Me2Si	2-(2-furyl)-5,9-diethyl-	2-(2-furyl)-5,9-diethyl-	Cl	A	B	C
		benzindenyl	benzindenyl
238b	Me2Si	2-(2-furyl)-azulenyl	2-(2-furyl)-azulenyl	Cl	A	B	C
239b	Me2Si	2-(4,5-dimethyl-2-furyl))-	2-(4,5-dimethyl-2-furyl))-	Cl	A	B	C
		azulenyl	azulenyl
240b	Me2Si	2-(5-trimethylsilyl-2-furyl))-	2-(5-trimethylsilyl-2-furyl))-	Cl	A	B	C
		azulenyl	azulenyl
241b	Me2Si	2-(2-furyl)-4-phenyl-azulenyl	2-(2-furyl)-4-phenyl-azulenyl	Cl	A	B	C
242b	Me2Si	2-methyl-4-phenyl-indenyl	2-(2-(5-methyl)-furyl)-4-phenyl-	Cl	A	B	C
			indenyl
243b	Me2Si	2-methyl-4-phenyl-indenyl	2-(2-(5-methyl)-furyl)-4-phenyl-	Cl	A	B	C
			indenyl
244b	Me2Si	2-methyl-4-(1-naphthyl)indenyl	2-(2-(5-methylfuryl))-4-(1-	Cl	A	B	C
			naphthyl)indenyl
245b	Me2Si	2-methyl-4-phenylindenyl	2-(2-(5-methylthienyl))-4-	Cl	A	B	C
			phenylindenyl

[0469] (iii) Examples include metallocene compounds classified into the bridged CpIndZr type; and out of compounds recited in the above-described literatures such as JP-A-6-87922, JP-A-8-92308, JP-A-9-87314, JP-A-7-224079 and JP-A-2005-336092, zirconium compounds belonging to formula (7b) and formula (9b).

[0470] Metallocene compounds classified into the bridged CpIndZr type are shown in Table b-13 to Table b-20.

[0471]

TABLE b-13
(iii) Bridged CpIndZr Type
No.	A1	A2	A3	A4
246b	Me2C	4-methyl-cyclopentadienyl	3-methyl-indenyl	Cl	A	B
247b	Me2C	4-tert-butyl-cyclopentadienyl	3-methyl-indenyl	Cl	A	B
248b	Me2C	4-tert-butyl-cyclopentadienyl	3-tert-butyl-indenyl	Cl	A	B
249b	Me2Si	4-methyl-cyclopentadienyl	3-methyl-indenyl	Cl	A	B
250b	Me2Si	4-tert-butyl-cyclopentadienyl	3-methyl-indenyl	Cl	A	B
251b	Me2Si	4-tert-butyl-cyclopentadienyl	3-tert-butyl-indenyl	Cl	A	B
252b	Me2C	4-methyl-cyclopentadienyl	3-methyl-indenyl	Me	A	B
253b	Me2C	4-tert-butyl-cyclopentadienyl	3-methyl-indenyl	Me	A	B
254b	Me2C	4-tert-butyl-cyclopentadienyl	3-tert-butyl-indenyl	Me	A	B
255b	Me2C	3-tert-butylcyclopentadienyl	2-methylindenyl	Cl	A	B	C	D
256b	Me2Si	2-methyl-4-phenyl-1-indenyl	2,3,5-trimethyl-1-	Cl	A	B	C	D
			cyclopentadienyl
257b	Me2Si	2-methyl-benz[e]indenyl	cyclopentadienyl	Cl	A	B	C	D
258b	Me2C	2-methylindenyl	cyclopentadienyl	Cl		B	C	D
259b	Me2Si	2-methyl-benz[e]indenyl	2-methylcyclopentadienyl	Cl	A	B	C	D
260b	Me2Si	2,3,4,5-tetramethyl-	2-methyl-4-phenyl-4H-1-	Cl	A	B	C	D
		cyclopentadienyl	azulenyl
261b	Me2Si	2,3,4,5-tetramethyl-	2-methyl-4-phenyl-5,6,7,8-	Cl	A	B	C	D
		cyclopentadienyl	tetrahydro-4H-1-azulenyl
262b	Me2Si	2,3,4,5-tetramethyl-	2,4-dimethyl-4H-1-azulenyl	Cl	A	B	C	D
		cyclopentadienyl
263b	Me2Si	2,3,4,5-tetramethyl-	2,4-dimethyl-5,6,7,8-	Cl	A	B	C	D
		cyclopentadienyl	tetrahydro-4H-1-azulenyl
264b	Me2Si	2,3,4,5-tetramethyl-	2-ethyl-4-phenyl-4H-1-azulenyl	Cl	A	B	C	D
		cyclopentadienyl
265b	Me2Si	2,3,4,5-tetramethyl-	2-ethyl-4-methyl-4H-1-azulenyl	Cl	A	B	C	D
		cyclopentadienyl
266b	Me2Si	cyclopentadienyl	2-(5-methyl-2-furyl)indenyl	Cl		B	C	D	E
267b	Me2Si	3-methylcyclopentadienyl	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
268b	Me2Si	3-ethylcyclopentadienyl	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
269b	Me2Si	3-phenylcyclopentadienyl	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
270b	Me2Si	3-tert-butylcyclopentadienyl	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
271b	Me2Si	3-(trimethylsilyl)-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl
272b	Me2Si	2,4-dimethylcyclopentadienyl	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E

[0472]

TABLE b-14
(iii) Bridged CpIndZr Type (continued)
No.	A1	A2	A3	A4
273b	Me2Si	2-methyl-4-phenyl-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl)
274b	Me2Si	2-methyl-4-(2-naphthyl)-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl
275b	Me2Si	2-methyl-4-tert-butyl-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl
276b	Me2Si	2-methyl-4-trimethyl-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		silylcyclopentadienyl
277b	Me2Si	2-ethyl-4-i-propyl-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl
278b	Me2Si	2,3,5-trimethyl-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl
279b	Me2Si	2,5-dimethyl-3-tert-butyl-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl
280b	Me2Si	2,3,4,5-tetramethyl-	2-(5-methyl-2-furyl)indenyl	Cl	A	B	C	D	E
		cyclopentadienyl
281b	Me2Si	cyclopentadienyl	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
			phenylindenyl
282b	Me2Si	3-methylcyclopentadienyl	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
			phenylindenyl
283b	Me2Si	3-ethylcyclopentadienyl	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
			phenylindenyl
284b	Me2Si	3-phenylcyclopentadienyl	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
			phenylindenyl
285b	Me2Si	3-tert-butylcyclopentadienyl	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
			phenylindenyl
286b	Me2Si	3-(trimethylsilyl)-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
287b	Me2Si	2,4-dimethylcyclopentadienyl	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
			phenylindenyl
288b	Me2Si	2-methyl-4-phenyl-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
289b	Me2Si	2-methyl-4-(2-naphthyl)-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
290b	Me2Si	2-methyl-4-tert-butyl-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
291b	Me2Si	2-methyl-4-trimethylsilyl-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
292b	Me2Si	2-ethyl-4-i-propyl-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
293b	Me2Si	2,3,5-trimethyl-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
294b	Me2Si	2,5-dimethyl-3-tert-butyl-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl
295b	Me2Si	2,3,4,5-tetramethyl-	2-(5-methyl-2-furyl)-4-	Cl	A	B	C	D	E
		cyclopentadienyl	phenylindenyl