Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – At least one aryl ring which is part of a fused or bridged...
Reexamination Certificate
2000-06-05
2002-02-26
Yoon, Tae H. (Department: 1714)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
At least one aryl ring which is part of a fused or bridged...
C524S322000, C524S504000, C525S069000, C525S073000
Reexamination Certificate
active
06350800
ABSTRACT:
FIELD OF THE INVENTION
The present invention relates to a high damping polymer gel composition with superior high-temperature stability, mechanical strength and moldability. The inventive composition is particularly useful as a molding material for various products.
BACKGROUND OF THE INVENTION
The polymerization of isobutylene and maleic anhydride is known, as is the polymerization of styrene and maleic anhydride, and the polymerization of methyl vinyl ether and maleic anhydride. These polymerization techniques are carried out by free radical initiation. Further, imidization between a maleic anhydride and a primary amine group is a commonly known chemical reaction.
It has long been recognized that two or more polymers may be blended together to form a wide variety of random or structured morphologies to obtain products that potentially offer desirable combinations of characteristics. However, it maybe difficult or even impossible in practice to achieve many potential combinations through simple blending because of some inherent and fundamental problem. Frequently, the two polymers are thermodynamically immiscible, which precludes generating a truly homogeneous product. While it is sometimes desirable to have a two-phase structure, the situation at the interface between these two phases very often leads to problems. The typical case is one of high interfacial tension and poor adhesion between the two phases. This interfacial tension contributes, along with high viscosities, to the inherent difficulty of imparting the desired degree of dispersion to random mixtures and to their subsequent lack of stability, giving rise to gross separation or stratification during later processing or use. Poor adhesion leads, in part, to the very weak and brittle mechanical behavior often observed in dispersed blends and may render some highly structured morphologies impossible.
SUMMARY OF THE INVENTION
The present invention is a polymeric gel composition comprising a polymer including an anhydride unit and an alkenyl unit; a crosslinking agent; a maleated polyalkylene; an extender; and an organic fatty acid.
According to one embodiment of this invention, a grafted “centipede” polymer of a maleated polyalkylene and a poly(alkenyl-co-maleimide) that is useful in producing high damping, soft materials with high service temperatures is provided. The centipede polymer can be formed by reacting polymeric constituents with a grafting agent, followed by mixture with an organic fatty acid.
It is an advantage of the invention to a produce centipede polymer composition that exhibits improved properties such as tensile strength, maximum elongation, tear strength, damping properties, high temperature compression set, and the like, with emphasis on the high temperature compression set. More particularly, the present inventive grafted poly(alkenyl-co-maleimide) copolymers combine with organic fatty acids to improve the tensile strength, tear strength, damping properties, and high-temperature compression set of the centipede polymer.
DETAILED DESCRIPTION OF THE INVENTION
The polymer gel composition of the present invention contains: 0.5-200 parts by weight of a poly(alkenyl-co-maleimide) having at least one maleated polyalkylene segment grafted thereto through at least one functional linkage formed by a cross-linking reaction with a grafting agent; and greater than 0 to about 100 parts by weight of an organic fatty acid.
The poly(alkenyl-co-maleimide) is a “centipede” polymer formed by imidizing a poly(alkenyl-co-maleic anhydride) with a primary amine. The “centipede” polymer has a high molecular weight spine connected with many relatively short side chains formed from the addition of the primary amines. The length of the main chain usually equals or is longer than the entanglement length, which is herein defined theoretically as an order of magnitude of 100 repeating units, while the length of the side chains is much smaller than the entanglement length.
The preferred alkenyl benzene contributed monomer units of the poly(alkenyl benzene-co-maleimide) “centipede” are any one or combination of styrene, &agr;-methylstyrene, 1-vinylnapthalene, 2-vinyl-napthalene, 1-&agr;-methylvinylnaphthalene, 2-&agr;-methylvinylnaphthalene, as well as alkyl, cycloalkyl, aryl, alkaryl, and aralkyl derivatives thereof, in which the total number of carbon atoms in the combined hydrocarbon is generally not greater than 12, as well as any di- or tri-vinyl aromatic hydrocarbons. The preferred vinyl aromatic hydrocarbons are either styrene or a-methylstyrene. The terms “alkenyl benzene” and “vinyl aromatic” are understood to be interchangeable as used herein.
The preferred R
1
R
2
ethylene contributed monomer units of the poly(R
1
R
2
ethylene-co-maleimide) “centipede” are any alkene such as ethylene, propylene, butylene, isobutylene, pentene, hexene, heptene, etc., as well as any di- or tri-alkene, with preference given to isobutylene.
The preferred alkyl vinyl ether contributed monomer units of the poly(alkyl vinyl ether-co-maleimide) “centipede” are any one or combination of methyl vinyl ether, ethyl vinyl ether, propyl vinyl ether, butyl vinyl ether, and any other alkyl vinyl ether wherein the number of carbons in the alkyl substituent is between 1 and 12. The preferred alkyl vinyl ether is methyl vinyl ether.
The poly(alkenyl-co-maleimide) described herein are subsequently graft-reacted through a difunctional linking or grafting agent to a maleated polyalkene to yield a maleated polymer having at least one polyalkylene segment grafted thereto through the at least one functional linkage thus formed. The alkylene moiety of the polyalkene may be, for example, ethylene, propylene, and mixtures of both. The preferred polyalkene is polypropylene.
The maleated polypropylene may be any of the conventionally known polypropylene compounds that are subsequently maleated by methods known in the art. The polypropylene grafted segment or segments have molecular weights M
w
of about 10,000 up to about 10,000,000, or higher, preferably about 20,000 to about 300,000.
The crystallinity, or tacticity, of the polypropylene may vary from being substantially amorphous to being completely crystalline, that is from about 10-100% crystallinity. Most typically, because of the extensive commercial use of isotactic polypropylene, the grafted polypropylene will be substantially crystalline, e.g., greater than about 90%. The polypropylene may be substantially free of ethylene. However, under certain circumstances small amounts of ethylene, on the order of less than about 10% by weight, may be incorporated. Furthermore, in certain instances the polypropylene contains small amounts of ethylene in copolymers known as “reactor copolymers”. Thus, it is within the scope of the invention that the grafted polypropylenes contain minor amounts of ethylene, both as part of the ethylene-propylene segments and as polyethylene segments.
The maleated polypropylene of this invention contains from about 0.01 wt. % incorporated maleic anhydride, based upon the weight of the maleated polypropylene, up to about 5 wt. %. Preferably, the maleic anhydride content will be from about 0.01 to about 2 wt. %, most preferably about 0.03 to about 0.2 wt. %. As will be apparent, unreacted polypropylene will also be present in the reaction mix as will minor amounts of reaction by-products, such as decomposed free-radical initiator compounds and low molecular weight free-radical products. These by-products are substantially removed, by methods known in the art, e.g. sparging with nitrogen or washing with water. Maleic anhydride may not be left in substantial amounts in the polymer without detrimental effects on the subsequent reaction of the poly(alkenyl-co-maleimide) with the maleated polypropylene.
The poly(alkenyl-co-maleimide) of the instant invention is formed by reacting a poly(alkenyl-co-maleic anhydride) in the presence of a mono-primary amine at a temperature from about 100° C. to about 300° C. and at a pressure from about slightly above vacuum to about 20 atmospheres, under substa
Foltz Victor J.
Hall James E.
Wang Xiaorong
McCollister Scott A.
Yoon Tae H.
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