Ethylene/alpha-olefin copolymer composition, graft modified ethylene/alpha-olefin copolymer composition, and multi-stage olefin polymerization process

Claim 2

An ethylene/α-olefin copolymer composition according to claim 1, wherein said at least two kinds of compounds (b) of Group IV transition metals of the periodic table containing a ligand having a cyclopentadienyl skeleton are: at least one kind of a transition metal compound represented by the following formula [b-I] : ML¹ X [b-I] wherein M is a transition metal atom selected from Group IVB of the periodic table, L¹ is a ligand coordinating to the transition metal atom M, at least two of the ligands L¹ are selected from a cyclopentadienyl group, a methylcyclopentadienyl group, an ethylcyclopentadienyl group and a substituted cyclopentadienyl group having at least one substituent group selected from a hydrocarbon group of 3 to 10 carbon atoms, and each of the other ligands L¹ is a hydrocarbon group of 1 to 12 carbon atoms, an alkoxy group, an aryloxy group, a trialkylsilyl group, a halogen atom or a hydrogen atom, and X is a valence of the transition metal atom M, and at least one kind of a transition metal compound represented by the following formula [b-II] : ML² X [b-II] wherein M is a transition metal atom selected from Group IVB of the periodic table, L² is a ligand coordinating to the transition metal atom, at least two of the ligands L² are substituted cyclopentadienyl groups having 2 - 5 substituent groups selected from a methyl group and an ethyl group, and each of the other ligands L² is a hydrocarbon group of 1 to 12 carbon atoms, an alkoxy group, an aryloxy group, a trialkylsilyl group, a halogen atom or a hydrogen atom, and X is a valence of the transition metal atom M.

Claim 3

An ethylene/α-olefin copolymer composition comprising: [A2] an ethylene/α-olefin copolymer in an amount of 20 to 90 % by weight, which is a copolymer of ethylene with an α-olefin of 3 to 20 carbon atoms and has such properties that: (A-i) the density is in the range of 0.850 to 0.980 g/cm³, and (A-ii) the intrinsic viscosity [η] as measured in decalin at 135 °C is in the range of 0.4 to 8 dl/g, (A-iii) the melt tension (MT (g)) at 190 °C and the melt flow rate (MFR) satisfy the relation MT > 2.2 × MFR -0.84 , (A-iv) the flow index (FI (l/sec)) defined by a shear rate which is given when a shear stress of molten copolymer at 190 °C reaches 2.4 × 10⁶ dyne/cm² and the melt flow rate (MFR) satisfy the relation FI < 150 × MFR, (A-v) the molecular weight distribution (Mw/Mn) measured by GPC is in the range of 1.5 to 4, and (A-vi) MT/(Mw/Mn) and FI/MFR satisfy the relation MT/(Mw/Mn) > 0.03 × FI/MFR - 3.0 with the proviso that when the value of 0.03 × FI/MFR - 3.0 is less than 0, it is taken as 0; and [B1] an ethylene/α-olefin copolymer in an amount of 10 to 80 % by weight, which is different from the ethylene/α-olefin copolymer [A2] and is obtainable by copolymerizing ethylene with an α-olefin of 3 to 20 carbon atoms in the presence of a catalyst for olefin polymerization comprising (a) an organoaluminum oxy-compound and (b') a compound of Group IV transition metal of the periodic table containing a ligand having a cyclopentadienyl skeleton, and which has such properties that: (B-i) the density is in the range of 0.850 to 0.980 g/cm³, and (B-ii) the intrinsic viscosity [η] as measured in decalin at 135 °C is in the range of 0.4 to 8 dl/g.

Claim 4

A graft modified ethylene/α-olefin copolymer composition obtainable by graft copolymerizing an ethylene/α-olefin copolymer composition with a polar monomer, wherein the ethylene/α-olefin copolymer composition comprises: [A3] an ethylene/α-olefin copolymer in an amount of 20 to 90 % by weight, which is obtainable by copolymerizing ethylene with an α-olefin of 3 to 20 carbon atoms in the presence of a catalyst for olefin polymerization comprising (a) an organoaluminum oxy-compound and (b') a compound of Group IV transition metal of the periodic table containing a ligand having a cyclopentadienyl skeleton, and which has such properties that: (A-i) the density is in the range of 0.850 to 0.980 g/cm³, and (A-ii) the intrinsic viscosity [η] as measured in decalin at 135 °C is in the range of 0.4 to 8 dl/g; and [B1] an ethylene/α-olefin copolymer in an amount of 10 to 80 % by weight, which is different from the ethylene/α-olefin copolymer [A3] and is obtainable by copolymerizing ethylene with an α-olefin of 3 to 20 carbon atoms in the presence of a catalyst for olefin polymerization comprising (a) an organoaluminum oxy-compound and (b') a compound of Group IV transition metal of the periodic table containing a ligand having a cyclopentadienyl skeleton, and which has such properties that: (B-i) the density is in the range of 0.850 to 0.980 g/cm³, and (B-ii) the intrinsic viscosity [η] as measured in decalin at 135 °C is in the range of 0.4 to 8 dl/g.

Claim 5

An ethylene copolymer composition comprising: [I] a graft modified ethylene/α-olefin copolymer composition obtainable by graft copolymerizing an ethylene/α-olefin copolymer composition with a polar monomer, said ethylene/α-olefin copolymer composition comprising: [A3] an ethylene/α-olefin copolymer in an amount of 20 to 90 % by weight, which is obtainable by copolymerizing ethylene with an α-olefin of 3 to 20 carbon atoms in the presence of a catalyst for olefin polymerization comprising (a) an organoaluminum oxy-compound and (b') a compound of Group IV transition metal of the periodic table containing a ligand having a cyclopentadienyl skeleton, and which has such properties that: (A-i) the density is in the range of 0.850 to 0.980 g/cm³, and (A-ii) the intrinsic viscosity [η] as measured in decalin at 135 °C is in the range of 0.4 to 8 dl/g; and [B1] an ethylene/α-olefin copolymer in an amount of 10 to 80 % by weight, which is different from the ethylene/α-olefin copolymer [A3] and is obtained by copolymerizing ethylene with an α-olefin of 3 to 20 carbon atoms in the presence of a catalyst for olefin polymerization comprising (a) an organoaluminum oxy-compound and (b') a compound of Group IV transition metal of the periodic table containing a ligand having a cyclopentadienyl skeleton, and which has such properties that: (B-i) the density is in the range of 0.850 to 0.980 g/cm³, and (B-ii) the intrinsic viscosity [η] as measured in decalin at 135 °C is in the range of 0.4 to 8 dl/g; and [II] polyolefin; wherein the weight ratio ([I] : [II]) of the graft modified ethylene/α-olefin copolymer composition [I] and the polyolefin [II] is from 1:99 to 99:1.

Claim 6

A multi-stage olefin polymerization process comprising: (1) preparing an ethylene/α-olefin copolymer [A1] by copolymerizing ethylene with an α-olefin of 3 to 20 carbon atoms in the presence of a catalyst for olefin polymerization (C1) comprising: (a) an organoaluminum oxy-compound, (b-I) at least one kind of a transition metal compound represented by the following formula [b-I] : ML¹ X [b-I] wherein M is a transition metal atom selected from Group IVB of the periodic table, L¹ is a ligand coordinating to the transition metal atom M, at least two of the ligands L¹ are selected from a cyclopentadienyl group, a methylcyclopentadienyl group, an ethylcyclopentadienyl group and a substituted cyclopentadienyl group having at least one substituent group selected from a hydrocarbon group of 3 to 10 carbon atoms, and each of the other ligands L¹ is a hydrocarbon group of 1 to 12 carbon atoms, an alkoxy group, an aryloxy group, a trialkylsilyl group, a halogen atom or a hydrogen atom, and X is a valence of the transition metal atom M, and (b-II) at least one kind of a transition metal compound represented by the following formula [b-II] : ML² X [b-II] wherein M is a transition metal atom selected from Group IVB of the periodic table, L² is a ligand coordinating to the transition metal atom, at least two of the ligands L² are substituted cyclopentadienyl groups having 2 - 5 substituent groups selected from a methyl group and an ethyl group, and each of the other ligands L² group is a hydrocarbon group of 1 to 12 carbon atoms, an alkoxy group, an aryloxy group, a trialkylsilyl group, a halogen atom or a hydrogen atom, and X is a valence of the transition metal atom M; and (2) preparing an ethylene/α-olefin copolymer [B1] by copolymerizing ethylene with an α-olefin of 3 to 20 carbon atoms in a different polymerizer from the polymerizer for the copolymerization reaction of the stage (1) in the presence of a catalyst for olefin polymerization (C2) comprising (a) an organoaluminum oxy-compound and (b') a compound of Group IV transition metal of the periodic table containing a ligand having a cyclopentadienyl skeleton.

Claim 7

A process according to claim 6, wherein the catalyst for olefin polymerization (C1) further comprises an organoaluminium compound (c) in addition to the organoaluminium oxy-compound (a), the transition metal compound (b-I) and the transition metal compound (b-II).

Claim 8

A process according to claim 6 or 7, wherein the catalyst for olefin polymerization (C1) is a solid catalyst in which the organoaluminium oxy-compound (a), the transition metal compound (b-I) and the transition metal compound (b-II) are supported on a carrier.

Claim 9

A process according to claim 8, wherein the catalyst for olefin polymerization (C1) is a prepolymerized catalyst obtainable by prepolymerizing an olefin on the solid catalyst component.

Claim 10

A process according to any one of claims 6 to 9, wherein the catalyst for olefin polymerization (C2) further comprises an organoaluminium compound (c) in addition to the organoaluminium oxy-compound (a) and the transition metal compound (b').

Claim 11

A process according to any one of claims 6 to 10, wherein the catalyst for olefin polymerization (C2) is a solid catalyst in which the organoaluminium oxy-compound (a) and the transition metal compound (b') are supported on a carrier.

Claim 12

A process according to any one of claims 6 to 11, wherein the catalyst for olefin polymerization (C2) is a prepolymerized catalyst obtainable by prepolymerizing an olefin on the solid catalyst component.

Claim 13

A composition according to claim 1 wherein the ethylene/α-olefin copolymer [A1] is obtainable using (a) an organoaluminium oxy-compound and (b) at least two transition metal compounds one of which has two ligands coordinating to the transition metal atom selected from a cyclopentadienyl group,a methylcyclopentadienyl group, an ethylcyclopentadienyl group and a substituted cyclopentadienyl group having at least one substituent group selected from a hydrocarbon group of 3 to 10 carbon atoms, and the other transition metal compound has two ligands co-ordinating to the transition metal atom, selected from substituted cyclopentadienyl groups having 2-5 substituent groups selected from a methyl group and an ethyl group.

Claim 14

A film comprising an ethylene/α-olefin composition as claimed in any one of claims 1 to 5.

Claim 15

A molded article comprising an ethylene/α-olefin composition as claimed in any one of claims 1 to 5.