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Miscible blends of ethylene copolymers with improved temperature resistanceRelated Patent Categories: Synthetic Resins Or Natural Rubbers -- Part Of The Class 520 Series, Natural Rubber Compositions Having Nonreactive Materials (dnrm) Other Than: Carbon, Silicon Dioxide, Glass Titanium Dioxide, Water, Hydrocarbon, Halohydrocarbon, Ethylenically Unsaturated Reactant Admixed With A Preformed Reaction Product Derived From: (a) At Least One Polycarboxylic Acid, Ester, Or Anhydride; (b) At Least One Polyhydroxy Compound; And (c) At Least One Fatty Acid Glycerol Ester, Or A Fatty Acid Or Salt Derived From A Naturally Occurring Glyceride, Tall Oil, Or A Tall Oil Fatty Acid, At Least One Solid Polymer Derived From Ethylenic Reactants Only, Polymer Mixture Of Two Or More Solid Polymers Derived From Ethylenically Unsaturated Reactants Only; Or Mixtures Of Said Polymer Mixture With A Chemical Treating Agent; Or Products Or Processes Of Preparing Any Of The Above MixturesMiscible blends of ethylene copolymers with improved temperature resistance description/claimsThe Patent Description & Claims data below is from USPTO Patent Application 20060148988, Miscible blends of ethylene copolymers with improved temperature resistance. Brief Patent Description - Full Patent Description - Patent Application Claims
[0001] This application is a Continuation-in-part of pending U.S. application Ser. No. 10/510,808 filed Oct. 6, 2004, pending U.S. application Ser. No. 10/997,283, filed Nov. 24, 2004, and pending U.S. application Ser. No. 11/191,808, filed Jul. 28, 2005. BACKGROUND OF THE INVENTION [0002] 1. Field of the Invention [0003] This invention relates to blended polyamide compositions, and to a process of preparing same. This invention relates to compositions comprising copolymers of ethylene and maleic anhydride or its functional equivalents and copolymers of ethylene with polar comonomers that provide products having improved properties. [0004] 2. Description of the Related Art [0005] Thermoplastic resins used as plastics in engineering applications can require additives to modify, that is, increase the impact resistance of said thermoplastic resins. U.S. Pat. No. 3,845,163 discloses blends of 60 to 85 weight percent polyamide and an acid-containing olefin polymer. U.S. Pat. No. 3,388,186 discloses a polyamide composition that includes an ethylene-containing grafted copolymer. U.S. Pat. No. 3,465,059 similarly discloses a polyamide composition that includes an ethylene-containing grafted copolymer. U.S. Pat. No. 3,668,274 discloses polycarbonamides that have been modified with an elastomeric phase and a rigid phase thermoplastic stage containing amine-reactive moieties. [0006] Maleic anhydride grafted polyolefins (maleated polyolefins) and ethylene copolymers are widely used as impact modifiers for engineering polymers, particularly for polyamide polymer resins. Maleated polyolefins can be the preferred modifiers for use with polyamide resins. U.S. Pat. No. 4,174,358 discloses copolymers of ethylene/maleic anhydride as tougheners for polyamides having a number average molecular weight of at least 5000. U.S. Pat. No. 5,346,963 describes the use of maleic anhydride-grafted substantially linear ethylene polymers and blends thereof with olefin polymers and also with non-olefin polymers such as polyamides. U.S. Pat. No. 6,008,297 describes polyamide compositions that include acid-grafted ethylene/alpha-olefin copolymers for improved low-temperature impact strength. [0007] The use of maleated polyolefins is not trouble-free, however. There are limitations with using maleated polyolefins as impact modifiers. For example, it can be difficult to reach a high level of grafting in a maleated polyolefin. Grafting, as conventionally practiced, involves the use of a free-radical initiator. To achieve higher levels of grafting, which can be desirable, it can be necessary to include the free-radical initiator in a higher concentration. Using the initiator at higher concentrations can cause undesirable side reactions, such as crosslinking and chain scission. For this reason, grafting of maleic anhydride at a concentration of greater than 2 weight % can be difficult and troublesome. In addition, controlling the quality and consistency of maleated polyolefins--particularly those having higher concentrations of maleic anhydride grafting--can be troublesome. By-products, unreacted monomers, and crosslinking can significantly detract from the quality of maleated polyolefins at any grafting level, but this can be more of a problem particularly as the grafting level increases. Further, the cost of producing maleated polyolefins with high maleic graft levels can be substantial. [0008] Ethylene copolymers that include reactive functional groups such as maleic anhydride can be readily obtained by a high-pressure free radical process. However, these copolymers generally are not good impact modifiers for polyamide polymer resins. [0009] It would be desirable to prepare an impact modifier for polyamide polymer resins that are effective tougheners for polyamide resins and do not have the problems associated with high levels of grafting in maleated polyolefins. SUMMARY OF THE INVENTION [0010] The present invention is a toughened polyamide composition, comprising (1) from about 50 to about 98 weight % of a polyamide polymer resin, and (2) from about 2 to about 50 weight % of an impact modifier composition comprising (a) from about 10 to about 50 weight % of a copolymer prepared from ethylene, a functional comonomer and optionally a third comonomer, wherein the functional comonomer is included in the range of from about 3 to about 15 weight % in the copolymer; and (b) from about 50 to about 90 weight % of an ethylene-based polymer. [0011] In another aspect, this invention provides a composition comprising: [0012] (c) a copolymer obtained from copolymerization of ethylene and maleic anhydride or its functional equivalent, in an amount from about 5 to about 95 weight % of the composition; and [0013] (d) at least one ethylene copolymer obtained from copolymerization of ethylene with a polar monomer wherein said polar comonomer is present in the copolymer in an amount of from 6 to 40 weight %, wherein said copolymer is selected from the group consisting of ethylene/vinyl acetate copolymers, ethylene/alkyl (meth)acrylate copolymers and ethylene/(meth)acrylate/carbon monoxide terpolymers, in an amount from about 5 to about 95 weight % of the composition. DETAILED DESCRIPTION OF THE INVENTION [0014] In one embodiment, the present invention is a composition useful as an impact modifier for polyamide polymer compositions. The composition comprises as one component a maleated polyolefin which is a copolymer of ethylene and maleic anhydride, or its functional equivalent. Such equivalents include derivatives of maleic anhydride such as maleic acid and/or salts thereof, maleic acid diesters, maleic acid monoesters, itaconic acid, fumaric acid, fumaric acid monoester, or mixtures of any of these. Maleated polyolefins also include E/X/Y terpolymers, wherein: E is ethylene; X is a monomer selected from the group consisting of vinyl acetate, (meth)acrylic acid, and/or derivatives thereof; and Y is maleic anhydride or its functional equivalent. Examples of monomers suitable for inclusion as component X are: (Meth)acrylic acid derivatives including acids, salts, esters, anhydrides, or other acid derivatives that are known to one of ordinary skill in the chemical arts. Preferred monomers suitable for inclusion as component X are (meth)acrylic acid esters of C.sub.1 to C.sub.4 alcohols. Preferred terpolymers include those wherein X is less than 10 weight %, and preferably less than 5 weight % of the terpolymer. Methyl acrylate and butyl acrylate are particular examples of acrylate monomers suitable for inclusion as component X. Suitable as Y components are: Maleic diesters or monoesters (wherein one carboxyl group of the maleic moiety is esterified and the other is a carboxylic acid, also known as maleic half-esters or alkyl hydrogen maleates) include esters of C.sub.1 to C.sub.4 alcohols, such as, for example, methyl, ethyl, n-propyl, isopropyl, and n-butyl alcohols. Preferably the maleated polyolefin includes maleic anhydride, maleic acid diesters, and/or maleic acid half-esters. More preferably the maleated polyolefin includes maleic anhydride and/or maleic acid half-esters. [0015] Other copolymers include: ethylene/maleic acid monoester/n-butyl (meth)acrylate; ethylene/maleic acid monoester/methyl (meth)acrylate; and ethylene/maleic acid mono-ester/ethyl (meth)acrylate terpolymers. For such copolymers, the alcohol moiety used in the maleic acid monoester comonomer can be the same as that used in the alkyl (meth)acrylate comonomer, or it can be different. Of particular note are ethylene/alkyl hydrogen maleate copolymers wherein the alkyl group is ethyl (E/EHM copolymers). [0016] Maleated polyolefins useful herein are obtained by a high pressure free radical polymerization process. A high pressure process suitable for use in the practice of the present invention is described, for example, in U.S. Pat. No. 4,351,931. [0017] The modifier composition comprises as a second component an ethylene-based polymer (base resin). The base resin can be: high density polyethylenes (HDPE); low density polyethylenes (LDPE); linear low density polyethylenes (LLDPE); ultra low density polyethylenes (ULDPE); copolymers of ethylene and alpha-olefin monomer using a metallocene catalyst (metallocene polyethylenes, or MPE); ethylene/propylene copolymers; or terpolymers such as ethylene/propylene/diene monomer (EPDM). Preferably, the base resin is a soft polymer. More preferably, the base resin is MPE, LLDPE and, most preferably, the base resin is MPE. [0018] Without being held to theory, MPE can be preferred in the practice of the present invention because of its substantially linear structure and narrow molecular weight distribution of MPE. MPE technology is capable of making lower density MPE with high flexibility and low crystallinity, which can be desirable as the second component of this invention. [0019] MPE technology is described in, for example, U.S. Pat. No. 5,272,236; U.S. Pat. No. 5,278,272, U.S. Pat. No. 5,507,475, U.S. Pat. No. 5,264,405, and U.S. Pat. No. 5,240,894. [0020] Suitable base resins can also include polar ethylene copolymers that are obtained from copolymerization of ethylene with a polar monomer. Such suitable polar copolymers include ethylene acrylate copolymers and ethylene vinyl acetate copolymers, including ethylene acrylic acid copolymers, ethylene methacrylic acid copolymers, salts derived from ethylene acrylic and/or methacrylic acid copolymers, ethylene acrylic ester copolymers, ethylene methacrylic ester copolymers, and/or mixtures of any of these. [0021] Preferred polar ethylene copolymers include ethylene/vinyl acetate copolymers and ethylene/alkyl (meth)acrylate copolymers. Preferred soft polymers for use as the base resin in the polyamide modifier composition are ethylene acrylate copolymers. Continue reading about Miscible blends of ethylene copolymers with improved temperature resistance... 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