Ethylene copolymer and aromatic vinyl graft copolymer and...

Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Mixing of two or more solid polymers; mixing of solid...

Reexamination Certificate

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C525S245000, C525S247000, C525S268000, C526S134000, C526S153000, C526S159000, C526S160000, C526S165000, C526S170000, C526S336000, C526S339000, C526S340000, C526S347000

Reexamination Certificate

active

06376614

ABSTRACT:

BACKGROUND OF THE INVENTION
1. Field of the Invention
The present invention relates to an ethylene copolymer and an aromatic vinyl graft copolymer and a method for producing the same. More particularly, the present invention relates to a novel ethylene copolymer which has a vinyl group in the molecular chain, which is endowed with excellent toughness and compatibility as well as heat resistance and chemical resistance, and which is useful as a heat-resistant elastomer and a raw material of a composite material; to a syndiotactic aromatic vinyl copolymer containing a macromer formed of the ethylene copolymer (hereinafter may be simply referred to as ethylene copolymer macromer) as a graft component; and to a method for producing the same effectively.
2. Related Art
Previously, the present inventors successfully developed a styrene polymer having a high syndiotacticity (Japanese Patent Application Laid-Open (kokai) Nos. 62-104818 and 63-241009). The styrene polymer having a syndiotactic structure is endowed with excellent heat resistance and chemical resistance, but does not exhibit sufficient toughness or elongation. In addition, it has poor compatibility with other resins; therefore its use has inevitably been limited.
In order to overcome this drawback, the present inventors succeeded in endowing the aforementioned styrene polymer having a syndiotactic structure with toughness by copolymerizing styrene with an olefin (Japanese Patent Application Laid-Open (kokai) Nos. 3-7705, 4-130114, and 4-300904).
However, these polymers are not necessarily satisfactory in terms of toughness, elongation, and compatibility with other resins. Moreover, they sometimes suffer from deterioration of heat resistance. Therefore, there has been demand for a technique which further improves properties such as toughness which maintaining excellent a heat resistance.
Furthermore, there has been demand for a technique to effectively improve toughness and elongation of fragile resins having high glass transition temperature such as typical polystyrene as well as polystyrene having a syndiotactic structure.
The thus-obtained random or block copolymer of styrene and an olefin suffers insufficient controllability of the copolymerization composition as well as a low copolymerization-modification ratio (i.e., percentage of modifier olefins in the resultant copolymer), leading to insufficient improvement in toughness, elongation, and compatibility with other resins.
There have also been proposed graft copolymers in which a styrene monomer is graft-copolymerized with a polymer having double bonds in side chains, as well as block copolymers in which a styrene monomer is block-copolymerized with a macromonomer having polymerization-active terminal vinyl groups (Japanese Patent Application Laid-Open (kokai) Nos. 05-247147 and 05-295056). However, the copolymers disclosed in the above publications exhibit an insufficient graft ratio, resulting in insufficient improvement in physical properties thereof.
In view of the foregoing, the present invention is directed to the provision of an ethylene copolymer which is remarkably useful as a macromonomer for obtaining a syndiotactic polystyrene graft copolymer having improved toughness, elongation, etc. or as a material for obtaining a compatibility-enhancing agent for a composition containing syndiotactic polystyrene and a rubber component, or a composition of typical polystyrene and a rubber component; the provision of a syndiotactic aromatic vinyl graft copolymer which is endowed with excellent toughness, elongation, and compatibility as well as heat resistance and chemical resistance, and is useful for a heat-resistant elastomer and a raw material of composite materials; and the provision of a method for producing the same in an effective manner.
SUMMARY OF THE INVENTION
The present inventors carried out extensive studies, and as a result, found that introduction of a styrenic vinyl group into the ethylene chain may provide an effective comonomer for obtaining a polystyrene graft copolymer, and that the polystyrene graft copolymer may serve as a compatibility-enhancing agent for a composition containing polystyrene and a rubber component.
The present inventors also found that a graft copolymer which is obtained from an aromatic vinyl monomer and the aforementioned ethylene copolymer serving as a macromer and which contains an aromatic-vinyl-monomer-derived chain having a stereospecificity of highly syndiotactic structure is endowed with excellent toughness, elongation, and compatibility as well as heat resistance and chemical resistance.
Furthermore, the present inventors found that ethylene copolymers are effectively obtained by using a specific catalyst. The present invention was accomplished based on these findings.
Specifically, the present invention provides:
(1) an ethylene copolymer comprising an aromatic vinyl monomer (A), ethylene (B), and a diene monomer (C) and having in the molecular chain a vinyl group attributed to a diene monomer, wherein recurrent units attributed to aromatic vinyl monomer (A) is 1-98 mol %, recurrent units attributed to ethylene (B) is 1-98 mol %, and recurrent units attributed to diene monomer (C) is 0.001-10 mol %.
(2) an ethylene copolymer comprising an aromatic vinyl monomer (A), ethylene (B), a diene monomer (C), and &agr;-olefin (D), and having in the molecular chain a vinyl group attributed to a diene monomer, wherein recurrent units attributed to aromatic vinyl monomer (A) is 1-98 mol %, recurrent units attributed to ethylene (B) is 1-98 mol %, recurrent units attributed to diene monomer (C) is 0.001-10 mol % and recurrent units attributed to &agr;-olefin (D) is 0-90 mol % (exclusive of 0).
(3) the ethylene copolymer described in either one of the above-described (1) or (2), wherein the diene monomer (C) is a diene having a styrenic vinyl group.
(4) a method for producing an ethylene copolymer recited in either one of the above-described (1) through (3), wherein the respective monomers are copolymerized through use of a catalyst formed of the following components (E) and (F):
(E) a transition metal compound; and
(F) an oxygen-containing compound (i) represented by the following formula (1) or (2):
wherein, each of R
1
through R
5
, which may be identical to or different from one another, represents a C1-C8 alkyl group; each of Y
1
through Y
3
, which may be identical to or different from one another, represents a Group 13 element; and a and b independently represent numbers between 0 and 50 inclusive, with the proviso that a+b is equal to or greater than 1;
wherein, each of R
6
and R
7
, which may be identical to or different from each other, represents a C1-C8 alkyl group; Y
4
and Y
5
, which may be identical to or different from each other, represents a Group 13 element; and c and d independently represent numbers between 0 and 50 inclusive, with the proviso that c+d is equal to or greater than 1: and/or a compound (ii) capable of forming an ionic complex through reaction with transition metal compound (E).
(5) a method for producing an ethylene copolymer recited in either one of the above-described (1) through (3), wherein the respective monomers are copolymerized through use of a catalyst formed of the following components (E), (F) and (G):
(E) a transition metal compound;
(F) an oxygen-containing compound (i) represented by the following formula (1) or (2):
wherein, each of R
1
through R
5
, which may be identical to or different from one another, represents a C1-C8 alkyl group; each of Y
1
through Y
3
, which may be identical to or different from one another, represents a Group 13 element; and a and b independently represent numbers between 0 and 50 inclusive, with the proviso that a+b is equal to or greater than 1;
wherein, each of R
6
and R
7
, which may be identical to or different from each other, represents a C1-C8 alkyl group; Y
4
and Y
5
, which may be identical to or different from each other, represents a Group 13 element; and c and d independently represent numbers between 0 and 50 i

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