Compatibilized resin blends and the preparation thereof

Details Compatibilized resin blends and the preparation thereof Compatibilized resin blends and the preparation thereof

2000-11-14

2002-10-22

Short, Patricia A. (Department: 1712)

Synthetic resins or natural rubbers -- part of the class 520 ser

Synthetic resins

Mixing of two or more solid polymers; mixing of solid...

C525S069000, C525S125000, C525S130000, C525S131000

Reexamination Certificate

active

06469099

ABSTRACT:

This invention relates to compatibilized resin blends of normally incompatible polymers and the preparation of such blends.
Compatibilizers for blends of certain polymers are known in the art. For example, U.S. Pat. No. 5,959,032 (Evans et al.) describes the preparation of a compatibilizer (for polypropylene and a thermoplastic polyolefin) which is the reaction product of an anhydride functionalized polypropylene and a polyetheramine.
JP Patent Application No. 3-231963 discloses a blend of a thermoplastic polyurethane and a polyolefin that is compatibilized with a polyolefin modified with carboxyl groups, anhydride groups, and/or epoxy groups. The compatibilized blend is reported to have high heat-resistance, high mechanical strength, and high wear resistance.
The compatiblized blends of the prior art generally suffer from having undesirably low weldline strength, which is important for applications such as automotive instrument panels or bumper beams, the manufacture of which generally requires multiple gate or complex injection molding design. Accordingly, it would be desirable to have available a compatibilizer that addresses this deficiency.
The present invention is a composition comprising a blend or reactive product of a) a thermoplastic polyurethane, and b) a compatibilizer, which is a first polymeric hydrocarbon that contains isocyanate-reactive groups or polyoxyalkylene groups.
In a second aspect, the present invention is a composition comprising a blend or reactive mixture of a) a thermoplastic polyurethane, and b) a compatibilizer, which is a first polymeric hydrocarbon that contains isocyanate reactive groups or polyoxyalkylene groups, and c) a second polymeric hydrocarbon, wherein the first and second polymeric hydrocarbons are each independently selected from the group consisting of polypropylene, high density polyethylene, low density polyethylene, linear low density polyethylene, substantially linear ethylene/&agr;x-olefin copolymers, polystyrene, poly-&agr;-methylstyrene, polyvinyltoluene, and ethylene-styrene interpolymer.
In a third aspect, the present invention is a method of preparing a compatibilizing composition comprising the step of compounding under reactive conditions a) a thermoplastic polyurethane, and b) a compatibilizer, which is a first polymeric hydrocarbon that contains isocyanate reactive groups.
In a first aspect the present invention is a composition comprising a blend or reactive product of a) a thermoplastic polyurethane, and b) a compatibilizer. The compatibilizer, which is a first polymeric hydrocarbon containing either isocyanate reactive groups or polyoxyalkylene groups, is advantageously prepared by contacting under reactive conditions a) a first polymeric hydrocarbon having pendant or incorporated amine-reactive groups with either b) a compound that contains at least one amine group and at least one isocyanate-reactive group; or c) a compound that contains an amine group and polyoxyalkylene group.
As used herein, the term polymeric hydrocarbon refers to a polyolefin, a polymer of an alkenyl aromatic hydrocarbon, or a polymer prepared from olefinic and alkenyl aromatic hydrocarbon monomers. The term isocyanate-reactive group refers to a group that reacts with an isocyanate group, preferably an amino group or hydroxyl group.
Examples of polyolefins include polypropylene, high density polyethylene (HDPE), low density polyethylene (LDPE), linear low density polyethylene (LLDPE), or substantially linear ethylene/&agr;-olefin copolymers such as those copolymers described in U.S. Pat. Nos. 5,272,236 and 5,278,272. Examples of polymers of alkenyl aromatic hydrocarbons include polymers of styrene, &agr;-methylstyrene, and vinyltoluene. An example of a polymer prepared from olefinic and alkenyl aromatic hydrocarbon monomers is ethylene-styrene interpolymer.
Amine-reactive groups can be made pendant to the backbone of the first polymeric hydrocarbon by grafting an ethylenically unsaturated amine-reactive compound onto the backbone of the polymeric hydrocarbon. Alternatively, amine-reactive groups can be incorporated into the backbone of the polymeric hydrocarbon by copolymerization of the olefin or alkenyl aromatic hydrocarbon monomer or both with an ethylenically unsaturated amine-reactive compound. Grafting is a preferred means of incorporating the amine-reactive groups into the polymeric hydrocarbon.
As used herein, the term “ethylenically unsaturated amine-reactive compound” refers to a compound that a) can be attached to the polymeric hydrocarbon by grafting or copolymerization and b) is chemically reactive with an amine. Similarly, the term “amine-reactive group” is used herein to refer to the remnant formed by grafting or copolymerization. Examples of ethylenically unsaturated amine-reactive compounds that can be grafted onto the polymeric hydrocarbon backbone or copolymerized with the olefin or alkenyl aromatic hydrocarbon monomer include ethylenically unsaturated carboxylic acids such as maleic acid, fumaric acid, itaconic acid, acrylic acid, methacrylic acid, and crotonic acid; acid anhydrides such as maleic anhydride and itaconic anhydride; vinyl benzyl halides such as vinyl benzyl chloride and vinyl benzyl bromide; alkyl acrylates and methacrylates such as methyl acrylate, ethyl acrylate, butyl acrylate, lauryl acrylate, methyl methacrylate, ethyl methacrylate, butyl methacrylate, and lauryl methacrylate; and ethylenically unsaturated oxiranes such as glycidyl acrylate, glycidyl methacrylate, and glycidyl ethacrylate. Preferred ethylenically unsaturated amine-reactive compounds include maleic anhydride, acrylic acid, methacrylic acid, glycidyl acrylate, glycidyl methacrylate, with maleic anhydride being more preferred. Polypropylene grafted with maleic anhydride is a more preferred modified polymeric hydrocarbon. An example of a commercially available modified polymeric hydrocarbon is EPOLENE™ PP 3003 wax (a trademark of Eastman Chemical Co), which is a propropylene wax that contains from about 0.5 to 1 weight percent grafted maleic anhydride units.
The degree of incorporation or grafting of the amine-reactive group is application dependent, but is preferably not more than 10 weight percent, more preferably not more than 5 weight percent, more preferably not more than 2 weight percent, and most preferably not more than 1 weight percent; and preferably not less than 0.01 weight percent, more preferably not less than 0.1 weight percent, and most preferably not less than 0.2 weight percent, based on the weight of the compatibilizer.
The hydroxylamine is a compound containing an amine group and at least one hydroxyl group, preferably only one hydroxyl group. The amine can be a primary or a secondary amine, and is preferably a primary amine. The polyamine is a compound that contains at least two amine groups, preferably only two amine groups. An example of a suitable class of hydroxylamines or polyamines is represented by the following formula:
where X is O or NH, where each R is independently H, —CH
3
, or —CH
2
CH
3
; and where x is from 0 to 50. The disclosure and preparation of hydroxyl amines can be found in U.S. Pat. Nos. 3,231,619, 4,612,335, and 4,888,446, which teachings are incorporated herein by reference. Examples of preferred oxyalkanolamines include 2-aminoethanol, 1-amino-2-propanol, 2-amino-1-propanol, 3-amino-1-propanol, 2-(2-aminoethoxy)ethanol, 1-amino-2-butanol, 2-amino-3-butanol, and polyoxyalkylene glycol amines. 2-Aminoethanol is a preferred alkanolamine.
The polyamine is a compound with at least two amine groups. Examples of suitable polyamines include &agr;-&ohgr; alkylene diamines such as ethylene diamine, 1,3-propylene diamine, 1,4-butylene diamine, and 1,6-hexylene diamine, as well as polyoxyalkylene diamines, commercially available as JEFFAMINE™ polyoxyalkylene diamines (a trademark of Huntsman Petrochemical). Where the amine-reactive groups pendant to the backbone of the first polymeric hydrocarbon are maleic anhydride groups, the compatibilizer prepared using polyamines or alkanolamines contains pendant

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