Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Polymers from only ethylenic monomers or processes of...
Reexamination Certificate
2000-08-16
2002-12-03
Pezzuto, Helen L. (Department: 1713)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Polymers from only ethylenic monomers or processes of...
C526S265000, C526S279000, C526S307800, C526S329200, C526S332000, C526S340000, C526S342000, C526S347000
Reexamination Certificate
active
06489425
ABSTRACT:
FIELD OF THE INVENTION
The present invention relates to a styrene/macromonomer random copolymer. More specifically, the present invention relates to a styrene/macromonomer random copolymer that has excellent melt flowability as well as good heat resistance, chemical resistance, dimensional stability, elongation, flexural strength, impact strength, compatibility, and electrical properties. The present invention includes a method of preparing the styrene copolymer. Also, the present invention relates to a styrene/styrene derivative/macromonomer random terpolymer and a method of preparing the terpolymer.
DESCRIPTION OF THE RELATED ART
In general, a styrene resin is prepared by radical polymerization. Since a styrene resin prepared by radical polymerization has an atactic structure as a whole, it has poor heat resistance and chemical resistance. A styrene resin with stereoregularity is prepared in the form of an isotactic structure or a syndiotactic structure. The former is polymerized by using a Ziegler catalyst and the latter is polymerized by using a uniform catalyst consisting of a titanium compound such as halogen titanium, alkoxy titanium, etc. with an alkylaluminoxane.
The styrene resin having a syndiotactic structure has good heat resistance and chemical resistance, but, on the other hand, it has poor impact strength. In order to overcome these shortcomings, methods of mixing a rubber, an inorganic filler, etc. have been attempted, such methods have limited usage. Further, since the melting point of the styrene resin is about 270° C. and the degradation temperature is 310° C., it is not easy to carry out such a process.
Recently, macromonomers with polymerization activity at the end of the chain have been developed and applied to various uses. The present inventors have developed a styrene/macromonomer random copolymer that has excellent melt flowability as well as good heat resistance, chemical resistance, dimensional stability, elongation, flexural strength, impact strength, compatibility, and electrical properties, which are required for engineering plastics. Further, the present inventors have developed a styrene/styrene derivative/macromonomer random terpolymer having excellent melt flowability as well as impact strength and other physical properties.
A feature of the present invention is the provision of a styrene random copolymer having excellent melt flowability, which is prepared by copolymerization of a styrene derivative monomer and a macromonomer and which is useful for engineering plastics having good heat resistance.
Another feature of the present invention is the provision of a styrene random copolymer prepared by copolymerization of a styrene derivative monomer and a macromonomer, which has good heat resistance, chemical resistance, dimensional stability, elongation, flexural strength, impact strength, compatibility, and electrical properties.
A further feature of the present invention is the provision of a method of preparing the styrene random copolymer prepared by copolymerization of a styrene derivative monomer and a macromonomer.
A further feature of the present invention is the provision of a styrene random terpolymer having excellent melt flowability, which is prepared by polymerization of a styrene monomer, a styrene derivative, and a macromonomer and which is useful for engineering plastics having good heat resistance.
A further feature of the present invention is the provision of a styrene random terpolymer prepared by polymerization of a styrene monomer, a styrene derivative, and a macromonomer, which has good heat resistance, chemical resistance, dimensional stability, elongation, flexural strength, impact strength, compatibility, and electrical properties.
A further feature of the present invention is the provision of a method of preparing the styrene random terpolymer by polymerization of a styrene monomer, a styrene derivative, and a macromonomer.
The above and the other features and advantages of this invention will be apparent from the ensuing disclosure and appended claims.
SUMMARY OF THE PREFERRED EMBODIMENTS
The styrene random copolymer according to the present invention is produced by copolymerization of a styrene monomer and a macromonomer, thus having at least two repeating units, the styrene derivative with a syndiotactic structure and the macromonomer. The macromonomer has polymerization activity via an ethylenically unsaturated group, such as a vinyl group, at the end of the chain. The repeating units of styrene derivative, and more particularly at least 50% syndiotacticity. The amount of macromonomer is about 0.1% to about 50% (0.1~50%) by weight based on the weight of the random copolymer. The melting point of the copolymer is 150~272° C., and the weight average molecular weight is in the range of about 50,000 to about 2,000,000 when it is measured by gel permeation chromatography.
Thus, according to one aspect of the present invention, a styrene random copolymer is provided that includes at least one unit of styrene derivative and at least one unit of macromonomer, the at least one unit of styrene derivative being polymerized from a styrene derivative monomer of formula (1), the at least one unit of macromonomer being polymerized from a macromonomer of formula (2).
In the forgoing formulae,
R
1
is selected from the group consisting of hydrogen, halogen, and alkyl groups with 1~20 carbon atoms, R
2
is at least one selected from the group consisting of saturated hydrocarbons with 1~20 carbon atoms, aromatic groups, and cycloalkyl groups with the proviso that R
2
is not —CO— or —CH
2
—C
6
H
4
—, R
3
is a saturated hydrocarbon group with 1~10 carbon atoms, X is at least one ion polymerizable monomer unit selected from the group consisting of monomers of formulae
R
4
, R
5
, R
6
, R
7
, R
8
, and R
9
are the same or different and are selected from the group consisting of hydrogen, halogen, alkyl groups with 1~20 carbon atoms, and alkoxy groups with 1~20 carbon atoms, R
10
, R
11
, R
12
, R
13
, R
16
, and R
17
are the same or different and are selected from the group consisting of alkyl groups with 1~20 carbon atoms, R
14
and R
15
are the same or different and are selected from the group consisting of hydrogen and alkyl groups with 1~20 carbon atoms, R
18
is selected from the group consisting of hydrogen and alkyl groups with 1~4 carbon atoms, R
19
is selected from the group consisting of alkyl groups with 1~4 carbon atoms, and l is the degree of polymerization for X and is an integer from about 10 to about 1,000.
The amount of the macromonomer is 0.1~50% by weight based on the weight of the random copolymer, and the weight average molecular weight of the random copolymer ranges from about 50,000 to about 2,000,000.
According to another aspect of the present invention, the styrene random copolymer is prepared by polymerization of a styrene derivative monomer and a macromonomer in the presence of a catalyst comprising a transition metal compound, more particularly a Group IV transition metal compound, and an alkylaluminoxane.
Further, the present invention includes a styrene random terpolymer that is copolymerized from a styrene monomer, a styrene derivative, and a macromonomer, thus having at least three repeating units, the two styrenes with a syndiotactic structure and the macromonomer. The macromonomer has a polymerization activity viaan ethylenically unsaturated group, such as a vinyl group, at the end of the chain. The repeating units of the styrene, and more particularly have at least 50% syndiotacticity. The amount of macromonomer is about 0.1 to about 50% by weight based on the weight of the random terpolymer. The melting point of the terpolymer is 150~272° C., and the weight average molecular weight is in the range of about 50,000 to about 5,000,000 when it is measured by gel permeation chromatography.
Thus, in accordance with an additional aspect of the present invention, there is provided a styrene random terpolymer comprising units of styrene monomer, units of styrene derivative, and units of macromonomer, th
Lyu Yi-Yeol
Yim Jin Heong
Yoon Keun-Byoung
Lee & Sterba, P.C.
Pezzuto Helen L.
Samsung Electronics Co,. Ltd.
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