# US 5,708,080 A · Graft modified ethylene/.alpha.-olefin copolymer

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- Number: US 5,708,080 A
- Document ID: US5708080A
- Status: Granted
- Kind: A
- Application number: 08/449,921
- Filed: 1995-05-25
- Granted: 1998-01-13
- Earliest claimed: 1992-11-19
- Assignees: Mitsui Petrochemical Industries, Ltd.
- Inventors: Toshiyuki Tsutsui; Ken Yoshitsugu; Mamoru Takahashi; Akira Todo; Seiji Ohta; Hajime Inagaki
- Web page: https://patentgrep.com/patent/US5708080A

## CPC

- C08F 10/00: Homopolymers and copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond
- C08F 210/16: Copolymers of ethene with alpha-alkenes, e.g. EP rubbers
- C08F 255/02: on to polymers of olefins having two or three carbon atoms
- C08F 255/04: on to ethylene-propylene copolymers {(C08F255/023 takes precedence)}
- C08F 255/08: on to polymers of olefins having four or more carbon atoms
- C08F 287/00: Macromolecular compounds obtained by polymerising monomers on to block polymers
- C08F 297/08: polymerising mono-olefins
- C08L 23/04: Homopolymers or copolymers of ethene
- C08L 23/0815: {with aliphatic 1-olefins containing one carbon-to-carbon double bond}
- C08L 51/06: grafted on to homopolymers or copolymers of aliphatic hydrocarbons containing only one carbon-to-carbon double bond
- C08F 4/65904: {in combination with another component of C08F4/64}
- C08F 4/65912: {in combination with an organoaluminium compound}
- C08F 4/65916: {supported on a carrier, e.g. silica, MgCl2, polymer}
- C08F 4/65922: {containing at least two cyclopentadienyl rings, fused or not}
- C08L 2205/02: containing two or more polymers of the same C08L -group
- C08L 2314/04: Philipps catalyst
- C08L 2314/06: Metallocene or single site catalysts
- C08F: MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08L: COMPOSITIONS OF MACROMOLECULAR COMPOUNDS (compositions based on polymerisable monomers C08F, C08G; artificial filaments or fibres D01F; textile treating compositions D06)

## Abstract

A graft-modified ethylene/.alpha.-olefin copolymer composition is prepared by graft copolymerizing an ethylene/.alpha.-olefin copolymer. The ethylene/.alpha.-olefin copolymer composition includes first and second ethylene/.alpha.-olefin copolymers. The copolymers are each prepared in the presence of a polymerization catalyst containing (a) an organoaluminum oxy compound and (b) for the first ethylene/.alpha.-olefin copolymer at least two kinds, and for the second ethylene/.alpha.-olefin copolymer one kind, of compounds of Group IV transition metals of the periodic table containing a ligand having a cyclopentadienyl skeleton. The ethylene/.alpha.-olefin copolymer composition may be blended with a polyolefin by mechanical or solution blending. The copolymer compositions have excellent moldability and heat stability properties and forms films having high transparency and mechanical strength.

## Claims

### Claim 1

A moldable graft modified ethylene/.alpha.-olefin copolymer composition obtained by graft copolymerizing an ethylene/.alpha.-olefin copolymer composition with a polar monomer, wherein the ethylene/.alpha.-olefin copolymer composition comprises:
(A1) an ethylene/.alpha.-olefin copolymer in an amount of 20 to 90% by weight, which is obtained by copolymerizing ethylene with an .alpha.-olefin of 3 to 20 carbon atoms in the presence of a catalyst for olefin polymerization comprising (a) an organoaluminum oxy-compound and (b) at least one kind of a transition metal compound represented by the following formula ›b-I!:
ML.sup.1.sub.x ›b-I!
wherein M is a transition metal atom selected from Group IVB of the periodic table, L.sup.1 is a ligand coordinating to the transition metal atom M, at least two of L.sup.1 are groups 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, L.sup.1 other than the (substituted) cyclopentadienyl 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
at least one kind of a transition metal compound represented by the following formula ›b-II!:
ML.sup.2.sub.x ›b-II!
wherein M is a transition metal atom selected from Group IVB of the periodic table, L.sup.2 is a ligand coordinating to the transition metal atom, at least two of L.sup.2 are substituted cyclopentadienyl groups having 2-5 substituent groups selected from a methyl group and an ethyl group, L.sup.2 other than the substituted cyclopentadienyl 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 which has such properties that:
(A-i) the density is in the range of 0.850 to 0.980 g/cm.sup.3,
(A-ii) the intrinsic viscosity (.eta.) as measured in decalin at 135.degree. C. is in the range of 0.4 to 8 dl/g; and
(A-iii) the melt tension (MT (g)) at 190.degree. C. and the melt flow rate (MFR) satisfy the relation
MT>2.2.times.MFR.sup.-0.84,
and
(B1) an ethylene/.alpha.-olefin copolymer in an amount of 10 to 80% by weight, which has a density and MFR different from the ethylene/.alpha.-olefin copolymer (A1) and is obtained by copolymerizing ethylene with an .alpha.-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/cm.sup.3, and
(B-ii) the intrinsic viscosity (.eta.) as measured in decalin at 135.degree. C. is in the range of 0.4 to 8 dl/g.

### Claim 2 (depends on 1)

The graft modified ethylene/.alpha.-olefin copolymer composition of claim 1 wherein the ethylene/.alpha.-olefin copolymer (A1) has the following properties:
(A-i) a density in the range of 0.890 to 0.935 g/cm.sup.3 ;
(A-ii) an intrinsic viscosity (.eta.) as measured in decalin at 135.degree. C., in the range of 1.25 to 8 dl/g; and
(A-iii) a melt tension (MT (g)) at 190.degree. C. and melt flow rate (MFR) satisfying the relation:
7.5.times.MFR.sup.-0.84 >MT>2.5.times.MFR.sup.-0.84 ;
and the ethylene/.alpha.-olefin copolymer (B1) has the following properties:
(B-i) a density in the range of from 0.910 to 0.960 g/cm.sup.3 ; and
(B-ii) intrinsic viscosity (.eta.), measured in decalin at 135.degree. C., in the range of 0.5 to 1.23 dl/g.

### Claim 3 (depends on 2)

The graft modified ethylene/.alpha.-olefin copolymer composition of claim 2 which comprises from 40 to 75% by weight of the ethylene/.alpha.-olefin copolymer (A1) and from 25 to 60% by weight of the ethylene/.alpha.-olefin copolymer (B1).

### Claim 4 (depends on 3)

The graft modified ethylene/.alpha.-olefin copolymer composition of claim 3 wherein the ethylene/.alpha.-olefin copolymer which is graft copolymerized with a polar monomer has the following properties:
(ii) a density in the range of from 0.890 to 0.95 g/cm.sup.3 ;
(iii) a melt flow rate (MFR) measured at a temperature of 190.degree. C. and with a load of 2.16 kg, in the range of 0.2 to 50 g/10 min.;
(iv) a melt tension (MT(g)) at 190.degree. C., and the melt flow rate (MFR) satisfying the relation:
MT>=2.2.times.MFR.sup.-0.84 ;
(v) a flow index (FI (1/sec)) defined by a shear rate which is given when a shear stress at 190.degree. C. reaches 2.4.times.10.sup.6 dyne/cm.sup.2 which is more than 130 times the melt flow rate (MFR);
(vi) the temperature (Tm (.degree. C.)) at which the endothermic curve of the composition measured by a differential scanning calorimeter shows a maximum peak which has the following relationship with the density (d):
TM<450.times.d-297;
(vii) the quantity fraction (W (percent by weight)) of an n-decane-soluble component at room temperature which has the following relationship with the density (d):
when
MFR.ltoreq.10 g/10 min.:
W<60.times.exp(-100 (d-0.88))+0.1;
and
when MFR>10 g/10 min.:
W<80.times.(MFR-9).times.exp (-100 (d-0.88))+0.1.