GB2289684A - Resin compositions - Google Patents

Description

1 1 1 1 2289684 RESINS The present invention relates to a resin

composition comprising an N- alkyl-substituted maleimide/olefin copolymer and a resin, which may have excellent heat resistance, rigidity, izod impact strength, weather resistance and dimensional resistance properties.

Recently, various high-performance resins have been actively developed with the progress of polymer-alloying technology. Developments in this field have rapidly enabled workers to plasticize materials which had not been previously plasticised. In particular, plasticization has been intensively studied in the field of the automobile, electric and electronic industries, for example, the plasticization of automobile bodies made of steels. Although an alloy of polycarbonate and ABS has been adopted once, one encounters problems with productivity, colour tone and the like because the alloy, having poor heat resistance, is coated off-line.

GE Company has developed an alloy of a polyamide and a polyphenylene oxide. Although this material has improved water absorption properties as well as improved change of dimension and physical properties when compared with the polyamide itself, there are many problems with inadequate physical properties, as well as low rigidity, poor weather resistance and the like which are due to defects in the amides.

As having low weather resistance and other good physical properties, polyesters such as a polybutylene terephthalate have been proposed to blend with a variety of resins such as a polyphenylene oxide, a polycarbonate and an elastomer. However, these blends do not provide the resins with satisfactory combined properties of heat resistance, rigidity, izod impact strength and the like.

on the other hand, maleimide copolymers with high 1 heat resistance have been studied f or various blending methods. For example, a method in which methyl methacrylate is copolymerized with an N- aromaticsubstituted maleimide is disclosed in Japanese Patent Publication No. 43-9753, Japanese Laid-Open Patent Nos. 61-141715, 61-171708 and 62- 109811, and a method in which styrene resins are copolymerized with an Naromaticsubstituted maleimide is disclosed in Japanese Laid-Open Patent Nos. 47-6891, 61-76512 and 61-276807. Although the resins obtained by these methods have higher heat resistance due to the increased content of N-aromaticsubstituted maleimides, there are still problems, such as they are very fragile, poor to process and colour easily. Thus these Naromatic-substituted maleimides are only blended in a small amount as heat resistance modifiers to acrylonitrile/butadiene/styrene (ABS) resin.

For preventing decrease in mechanical strength of the resins by increasing the amount of maleimide units, for example, a method for graftpolymerizing phenylmaleimide and styrene to a rubber-like material, or a method for kneading them with a rubber-like material is described in, for example, Japanese Laid-open Patent Nos. 58-206657, 59-11322 and 59-49255. Since the heat resistance and rigidity of the resins were decreased by introducing rubber components using these methods to increase their izod impact strength, it is difficult to satisfy heat resistance, izod impact strength and rigidity all at the same time. Furthermore, use of resins with light colours is limited because of colouring moulded obj ects. Compositions of such materials and polyamide resins are also described in Japanese Laid-Open Patent Nos. 62-59647 and 62-179546, though again it proved difficult to satisfy heat resistance, izod impact strength and rigidity characteristics all at the same time.

2 i t, Although N-alkyl-substituted maleimide/olefin copolymers are interesting polymers which have properties such as good heat resistance and weather resistance, high rigidity, and practical mechanical strength, it is desirable to improve the izod impact strength of these resins, and an improvement in changes in physical properties and change in dimension caused by water absorption is also desired. Japanese Patent Publication No. 49-12576 describes a resin composition of maleimideolef in compound, a simple blend, that is not made by a reaction (interaction), so that it improves a little in flexural stiffness and izod impact strength.

Accordingly, one object of the present invention is to provide resin compositions that may have excellent heat resistance, rigidity, izod impact strength, weather resistance, dimensional resistance and the like.

As a result of intensive research to solve this problem, the Applicants have found a resin comprising an N-alkyl-substituted maleimide/olefin copolymer and a specified resin, which can satisfy this objective.

Thus, the invention relates to a (e.g. heat resistant) resin comprising component I repeating units and component II repeating units, component I having the general formula:

-HC-CH0 = C C = 0 N R1 (I) wherein R, represents a C,-,. alkyl group or a C,-.2 cycloalkyl group; and 3 component II has the general formula:

R3 1 -CH-C- (II) 1 1 Ii R2 R4 wherein R2 represents a hydrogen atom or a C,-, alkyl group, each of R3 and R4 independently representing a C,-,, group.

This resin (hereinafter referred to as resin a) preferably has a weight average molecular weight (suitably converted into that of polystyrene) of from 1,000 to 5,000,000.

Preferably the resin comprises from 30 to 98% of repeating units 1, and from 70 to 2% of repeating units of the formula II. Although not essential, it is preferred that the polymer has repeating units of component I and component II totalling at least 90%, preferably at least 95%, and optimally at least 99%. Thus, while it is anticipated that the polymer may contain any repeating units of formulae I and II (i.e. their amounts total 100%) this is by no means essential and the resins and resin compositions of the invention are to be construed as additionally including other polymers and repeating units of different formulae to those of components I and II. However, components I and II preferably constitute no more than 75 (molar) of resin (a).

Resin a) may be additionally combined with substance b), substance b) being an olefin resin, a modified elastomer, a polyamide resin and/or a polyester resin. Suitably the ratio of a/b is from 5/95 to 99/1 by weight. Such a composition may additionally comprise an elastomer, such as up to 40% by weight.

Thus, according to a first aspect of the present 4 z invention, there is provided an (e. g. heat-resistant) resin composition comprising:

(a) a resin in which 40 to 85 mole % of component (I) constitutes the whole polymer and 60 to 15 mole 0i of component (I1) constitutes the whole polymer; preferably the weight-average molecular weight (converted into that of polystyrene) is from 1 x 103 to 5 X 106; and b) an olefin resin; the a/b content being from 5/95 to 99/1 by weight; component 1 having the generaf formula:

_HC-CH- 11 '114 - - 0 = C C = 0 G1) N 1 R, wherein R, represents a C,_,a alkyl group or a C3-12 cycloalkyl group; and component II has the general formula:

R 1 3 -CH-C- A t R2 R' (11) wherein R2 represents a hydrogen atom or a C,-, alkyl group and each Of R3 and R4 independently represents a C,-, alkyl group.

The amounts of components 1 and 11 do not necessarily total 100%, although they may be. Other polymers and modified units of I and 11 (e.g. at up to 25%) can be included if necessary.

According to a second aspect of the present invention, there is provided a resin composition comprising:

a) resin (a) previously mentioned in the first aspect i c) b) a modified elastomer; the a/b content being from 5/95 to 99/1 as a weight ratio.

A third aspect relates to a resin composition comprising:

a) from 1 to 99% by weight of resin (a) previously mentioned for the first aspect; b) from 1 to 99% by weight of a polyamide resin; and from 0 to 40% by weight of an elastomer.

A fourth aspect relates to a resin composition comprising:

a) from 1 to 99% by weight of resin (a) previously mentioned for the first aspect; b) from 1 to 99% by weight of a polyester resin; and c) from 0 to 40% by weight of an elastomer.

As will become apparent from the following Examples, the resin compositions of the present invention may have excellent heat resistance, izod impact strength, rigidity and dimensional resistance and good mechanical strength, and so can be usefully applied in the technical fields of automobiles, electrics and electronics, aeronautics and shipping, residential, and medical, food and similar industries.

The resin compositions of the present invention may have combined excellent heat resistance, rigidity, izod impact strength, weather resistance and dimensional resistance.

The resin a) present in the resin composition of the present invention can be prepared by radical polymerization of an N-alkyl substituted maleimide and an olefin.

Examples of suitable N-alkyl-substituted maleimides include Nmethylmaleimide, N-ethylmaleimide, N-npropylmaleimide, N-ipropylmaleimide, N-n-butylmaleimide, N-i-butylmaleimide, N-sbutylmaleimide, N-t- 6 butylmaleimide, N-n-pentylmaleimide, N-n-hexylmaleimide, N-n-heptylmaleimide, N-n-octylmaleimide, laurylmaleimide, N-stearylmaleimide, Ncyclopropylmaleimide, Ncyclobutylmaleimide, Ncyclohexylmaleimide and the like; and preferably N methylmaleimide, N-ethylmaleimide, N-isopropylmaleimide or Ncyclohexylmaleimide. one or more compounds of such can be used in combination.

Examples of suitable olefins include isobutene, 2methyl - 1-butene, 2 methyl -1-pentene, 2-methyl-l-hexene, 1-methyl-l-heptene. 1-isooctene, 2methyl-l-octene, 2ethyl - 1-pentene, 2 -methyl -2 -butene, 2 -methyl -2 pentene, 2 -methyl -2 -hexene and the like, and preferably isobutene. One or more of these compounds can be used in combination.

The content of the component (I) is suitably from 30 to 98 mole %,, preferably from 40 to 85 mole %, and optimally from 45 to 75 mole %. When the content of the component (I) is more than 98 mole %, fragile polymers may result. In contrast. if the content is less than 30 mole %, polymers with decreased heat resistance may be prepared. The content of the components may be appropriately determined by adjusting the amount of these compounds in the reaction.

The resin a) may preferably have been modified with certain reactive groups. Examples of these reactive groups include carboxylic acids and derivatives thereof, acid anhydrides, epoxy, amino, hydroxyl, thiol, (e.g. Cl-,) alkoxysilyl and isocyanate groups. The content of such reactive groups is suitably from 0 to 25 mole %, preferably from 0.01 to 20 mole %, and optimally from 0. 02 to 5 mole %. These f igures thus ref er to the percentage of repeating units possessing a repeating unit. When the content of any reactive groups exceeds than 25 mole %, an undesirable resin may result with 7 decreaged heat otability and ratchanical gtrength.

Thus, the resin may comprise repeating units of formula I, formula II and repeating units which are modified units of formulae I and/or II, these three types of units preferably totalling 100%. The modified units preferably constitute from 0 to 25% of the resin.

These modified resins can be prepared by copolymerization or graft polymerization of the following monomers: for example, maleic anhydride, citraconic anhydride, itaconic anhydride, acrylic acid, methacrylic acid, itaconic acid, glycidyl acrylate, glycidyl methacrylate, aminoethyl acrylate, aminoethyl methacrylate, hydroxyethyl acrylate, hydroxyethyl methacrylate, triethoxysilylpropyl methacrylate, triethoxysilylpropyl methacrylate, aminostyrene, allylamine and the like.

Furthermore, reactive groups can be introduced in to polymers at their ends using initiators with reactive groups such as 4,41-azobis(4cianovaleric acid), 2,,21azobis(2-cianopropanol) and 2,21azobisisobutylamide, or using chain transfer agents with reactive groups such as mercaptoacetic acid and mercaptopropionic acid.

As will be described, if the resin a) is obtained by subjecting a copolymer of maleic anhydride and an olefin to imidation, adjustment of the degree of imidation can result in acid anhydride units remaining.

These reactive groups can be introduced depending on the reactive groups of the specified resin used.

If necessary, other monomers may be subjected to copolymerization without departing from the scope of the present invention. Examples of other vinyl monomers include styrene, a-methylstyrene, vinyltoluene, 1, 3butadiene, isoprene and halogen-substituted derivatives thereof; methacrylic esters such as methyl methacrylate, ethyl methacrylate, cyclohexyl methacrylate, phenyl 8 methacrylate and benzyl methacrylate; acrylic esters such as methyl acrylate, ethyl acrylate, butyl acrylate, cyclohexyl acrylate, phenyl acrylate and benzyl acrylate; vinyl esters such as vinyl acetate and vinyl benzoate; vinyl ethers such as methyl vinyl ether, ethyl vinyl ether, propyl vinyl ether and butyl vinyl ether; and one or more of the compounds vinyl chloride, vinylidene chloride, maleic anhydride, Nphenylmaleimide, Ncarboxyphenylmaleimide, acrylonitrile, ethylene, propylene, 1-butene, 2-butene and 1-hexene.

For polymerization of these monomers, any publicly for example, bulk polymerization, solution polymerization, suspension polymerization and emulsion polymerization can be employed.

Examples of polymerization initiators include organic peroxides such as benzoyl peroxide, lauryl peroxide, octanoyl peroxide, acetyl peroxide, dit-butyl peroxide, t-butyl cumyl peroxide, dicumyl peroxide, tbutyl peroxyacetate and t-butylperoxy benzoate; or azo initiators such as 2,21azobis(2,4-dinethylvaleronitrile), 2,21-azobis(2-butylonitrile), 2, 21azobisisobutylonitrile, dimethyl-2,21-azobisisobutylate and 1,11azobis(cyclohexane-l-carbonitrile).

Examples of solvents which can be used in a solution polymerization method include benzene, toluene, xylene, ethylbenzene, cyclohexane, dioxane, tetrahydrofuran, acetone, methyl ethyl ketone, dimethylformamide, isopropyl alcohol, butyl alcohol and the like.

The polymerization temperature can be appropriately adjusted depending on the decomposition temperature of the initiators, but it is usually preferred to be between 40 and 1500C.

The resins of the invention may be also obtained by subjecting resins resulting from copolymerization of known method for polymerization, 9 maleic anhydride and olef ins to imidation with alkylamine and the like. Imidation can be performed by melting, for example, a maleic anhydride/isobutene copolymer, or dissolving or dispersing the copolymer in an alcoholic solvent such as methanol, ethanol and propanol, or an aromatic solvent such as benzene and toluene; then reacting this with a primary amine such as methyl amine and the like, suitably at a temperature of 100 to 3500C.

The weight-average molecular weight (MW) of the resin prepared can be determined by gel permeation chromatography (GPC). The molecular weight of the maleimide copolymer is suitably from 1 X 103 to 1 X 106, pref erably from 1 x 10-5 to 1 X 106 or less. I f the molecular weight is more than 5 x 106, the resulting resin may tend to have poor moulding properties; and if the figure is less than 1 X 103, the resin has a tendency to become fragile.

Since N-alkyl-substituted maleimide/olefin copolymers are materials which may have excellent heat resistance, good weather resistance, practical mechanical strength and very high rigidity, compositions with even better physical properties can be obtained by use of those materials.

Examples of olef in resins that can be used in the resin compositions of the present invention include polyethylene, polypropylene, poly-4-methyll-pentene and modified derivatives thereof. The polyethylene preferably used in the compositions of the present invention, which is a resin mainly composed by ethylene units, is a polymer in which suitably 60 mole or more, preferably 80 mole % or more, and optimally 90 mole or more of the ethylene units constitute the whole resin.

Polyethylenes which can be used as olefin resins in the present invention may be subjected to copolymerization or graft polymerization with other unsaturated monomers capable of copolymerization, for example at-olefins such as propylene, 1-butene and 1hexene; vinyl ethers; vinyl esters such as vinyl acetate and vinyl propionate; acrylic esters; methacrylic esters; acrylonitrile and the like, the amounts of which are in the ranges of suitably from 0 to 40 mole %, preferably from 0 to 25 mole %, and optimally from 0 to 15 mole %.

These polyethylenes may preferably be modified by various reactive groups, examples of which include acid anhydrides, carboxylic acids and derivatives thereof, and hydroxyl, thiol, amino, epoxy, alkoxysilyl and isocyanate groups. Those modifications can be performed by publicly known copolymerization, graft polymerization and similar methods using, for example, maleic anhydride, citraconic anhydride, itaconic anhydride, acrylic acid, methacrylic acid, hydroxyethylmethacrylate, aminoethyl methacryl ate, glycidyl methacrylate, glycidyl acrylate and the like. The amount of the modified polyethylene possessing these reactive groups is suitably from 0 to 25 mole %, preferably from 0.01 to 15 mole %, and optimally 0.02 to 5 mole %.

The preferred polypropylenes which can be used as olefin resins in the present invention are those containing 80 mole % of polypropylene units in the whole resin, and may be subjected to copolymerization or graft polymerization with other unsaturated monomers capable of copolymerization, for example, a-alefins such as ethylene, 1-butene and 1hexene; vinyl ethers; vinyl esters such as vinyl acetate and vinyl propionate; acrylic esters; methacrylic esters; acrylonitrile and the like, the amounts of which are preferably within the range of from 0 to 20 mole %.

These polypropylenes may be modified by various reactive groups, examples of which include acid anhydrides, carboxylic acids and derivatives thereof, and hydroxyl, amino, epoxy, alkoxysilyl groups and the like. Those modifications can be performed by publicly known copolymerization, graft polymerization and similar methods using, f or example, maleic anhydride, acrylic acid, methacrylic acid, hydroxyethyl methacrylate, aminoethyl methacrylate, glycidyl methacrylate and the like, preferably a modified polypropylene grafted with maleic anhydride, acrylic acid, etc. The amount of the modified polypropylene with these reactive groups is suitably from 0 to 20 mole %, preferably from 0.01 to 5 mole %. Further, a poly-4-methyl-l-pentene which can be used as an olefin resin in the present invention, namely a polymer mainly composed by 4 -methyl -1pentene units, may be also modified by various reactive groups.

The resin composition of the present invention may also include third component capable of reacting with any reactive groups of the maleimide copolymer and/or olef in. Examples of this include maleic anhydridemodified maleimide copolymer/maleic anhydride-modified polyethylene/diamines such as diaminodiphenyl ether and the like or polyamine compounds such as a polyallylamine and the like, and carboxylmodified maleimide copolymer/ carboxyl-modified polypropylene/diepoxy compounds or epoxy resins such as diglycidyl phthalate and the like. In the resin compositions of the present invention, the content (weight ratio) of the resin a) N-alkylsubstituted maleimide/olefin copolymer and the resin b) polyolefin is suitably 5-99:95-1, preferably 50-99:50-1, and optionally 70-98:30-2.

Being modified substance of viscoelastic elastomers having glass transition temperatures of 100C or less, the modified elastomers in the second aspect of the present invention are preferably, but not limited to, modified substances such as diene elastomers and hydrogenated elastomers thereof, olefin elastomers, acrylic 12 z 0 elastomers, silicone elastomers, fluorine elastomers, urethane elastomers, ester elastomers and amide elastomers. These elastomers may be modified by various reactive groups, examples of which include acid anhydrides, carboxylic acids and derivatives thereof, and hydroxyl, amino, epoxy, alkoxysilyl, isocyanate groups and the like, such as maleic anhydride, citraconic anhydride, itacanic anhydride, acrylic acid, methacrylic acid, itaconic acid, fumaric acid, glycidyl acrylate, glycidyl methacrylate, 2- aminoethyl acrylate, 2aminoethyl methacrylate, 2-hydroxyethyl acrylate, 2hydroxyethyl methacrylate, triethoxysilylpropyl acrylate, triethoxysilylpropyl methacrylate, allylamine, etc. These modifications can be performed by a publicly known method such as copolymerization or graft polymerization.

Thus, examples of modified elastomers include acid anhydride-modified substances, epoxy-modified substances or hydroxy-modified substances of diene elastomers such as a polybutadiene, a styrene/butadiene rubber, an acrylonitrile/butadiene rubber, an acrylonitrile/styrene/ butadiene rubber, methyl methacrylate/styrene/butadiene, an isopropylene rubber and a chloroprene rubber; acid anhydride-modified substances, epoxy-modified substances or carboxy-modified substances of hydrogenated diene elastomers; acid anhydride-modified substances, epoxymodified substances, carboxy-modified substances or hydroxy-modified substances of olefin elastomers such as an ethylene/propylene (ethylidene norbornene) rubber, a butyl rubber, an ethylene/vinyl acetate rubber and ethylene/methyl acrylate; acid anhydride-modified substances, epoxy-modified substances or amino-modified substances of an acrylic rubber mainly composed of ethyl acrylate; epoxy-modified substances, substances or amino-modified substances of a polysiloxane; and the like.

13 hydroxy-modified Selection of these elastomer components may provide the resin composition with physical properties such as low temperature izod impact strength, oil resistance, desirable moulding properties and weather resistance. The use of modified substances of diene elastomers may provide low temperature izod impact strength, and the modified substances of olefin elastomers and acrylic elastomers may provide weather resistance and izod impact strength.

The reactive group content of the whole elastomer is suitably from 0.001 to 30 mole %, preferably from 0.01 to 20 mole %, and optimally from 0.05 to 5 mole %.

The resin composition of the present invention may also include a third component capable of reacting with the reactive group of the maleimide copolymer and/or modified elastomer. Examples of these include maleic anhydride-modified maleimide copolymer/maleic anhydridemodified elastomer/diamino compounds such as diaminodiphenyl ether and the like, and hydroxy-modified maleimide copolymer/hydroxy-modified elastomer/diepoxy compounds such as diglycidyl phthalate and the like.

The polyamide resins used in the resin compositions of the present invention can be polyamides obtained from ring opening polymerization of lactams such as e-caprolactam and g-dodecalactam; polyamides obtained from amino acids such as 6-aminocapronic acid, 11aminoundecanoic acid and 12aminododecanoic acid; polyamides obtained from aliphatic, cycloaliphatic and aromatic diamines such as ethylenediamine, tetramethylenediamine, hexamethylenediamine, undecamethylenediamine, dodecamethylenediamine, 2, 2t4trimethylhexamethylenediamine, 1,3- or 1,4bis(aminomethyl)cyclohexane, bis(4,41aminocyclohexyl)methane, methaxylenediamine and paraxylenediamine, and aliphatic, cycloaliphatic and 1 aromatic dicarboxylic acid such as adipic acid, suberic acid, sebacic acid, dodecane diacid, 1,4cyclohexanedicarboxylic acid, isophthalic acid and terephthalic acid, and copolymers and mixtures thereof. Among them, nylon 6, nylon 66, nylon 610, nylon 612, nylon 11, nylon 12, nylon 46 are particularly useful.

In general, publicly known melt polymerization, solution polymerization, solid phase polymerization and a combination of these polymerization methods be adopted to polymerizing these polyamides. Generally, the molecular weight of the polyamides is preferably, but not limited to, 10000 or more.

Some elastomers are preferably blended in to the resin compositions of the present invention. The elastomers of macromolecular compounds having glass transition temperatures of 100C or less, which can be used in resin compositions of the present invention, include olefin elastomers, diene elastomers and hydrogenated elastomers thereof, acrylic elastomers, silicone elastomers, fluorine elastomers and the like. The olefin elastomers and acrylic elastomers are preferred for their weather resistance, mechanical strength and the like.

Examples of olefin elastomers include butyl rubber and ethylene elastomers. Suitably the butyl rubber is mainly composed by a polyisobutylene. The ethylene elastomer, a polyethylene and copolymer thereof, is preferably composed of 50 mole % or more, preferably 75 mole % or more of ethylene units in the whole elastomer. Examples of other unsaturated monomers capable of copolymerizing with ethylene include aolefins such as propylene, 1-butene and 1-hexene, vinyl ethers, vinyl esters such as vinyl acetate and vinyl propionate, acrylic esters, methacrylic esters and acrylonitrile. They may be formed by copolymerization or graft polymerization according to publicly known methods.

The acrylic elastomer may be mainly composed of acrylic esters such as methyl ester, ethyl ester or butyl esters of acrylic acid. Examples of other components capable of copolymerizing with them include aromatic monomers such as styrene, methacrylic esters, vinyl acetate and the like.

These elastomers are preferably modified by various reactive groups. Examples of reactive groups include acid anhydrides, carboxylic acids and derivatives thereof, and hydroxyl, thiol, amino, epoxy, alkoxysilyl, isocyanate groups and the like. Those modifications can be performed by publicly known copolymerization, graft polymerization and similar methods using, for example, maleic anhydride, citraconic anhydride, itaconic anhydride, acrylic acid, methacrylic acid, itaconic acid, hydroxyethyl methacrylate, aminoethyl methacrylate, glycidyl methacrylate, glycidyl acrylate, 3(triethoxysilyl)propyl methacrylate and the like. The amount of the modified elastomer with these reactive groups is suitably from 0 to 25 mole %, preferably from 0.01 to 15 mole %, and optimally from 0.02 to 5 mole %.

Further practical examples of these elastomers include ethylene/propylene rubber and acid anhydridemodified derivatives thereof, a carboxylic acidmodified derivative, a glycidyl methacrylate-modified derivative, an ethylene/acrylic acid copolymer, an ethylene/glycidyl methacrylate copolymer, an ethylene/ethyl acrylate/glycidyl methacrylate copolymer, an ethylene/ethyl acrylate/maleic anhydride copolymer, an ethylene/vinyl acetate/maleic anhydride copolymer, an ethyl acrylate/glycidyl methacrylate copolymer, and ethyl acrylate/butyl acrylate/maleic anhydride copolymer and the like.

In the resin compositions of the present invention, the content (weight ratio) of the N-alkyl -substituted 16 1 maleimide/olefin copolymer, the polyamide resin an elastomer is suitably from 1-99:99-1:0-40, preferably from 5-95:95-5:0-30, and optimally from 10-75:90-25:1-25. When the content of the maleimide copolymer is 1% by weight or less, a resin with poor heat resistance and low rigidity may be obtained. On the other hand, if the elastomer content is 40% by weight or more, a resin with a decreased heat resistance and rigidity may be obtained.

Examples of polyester resins that can be used in the resin composition of the present invention include polybutylene terephthalate, polyethylene terephthalate, polyacrylates, liquid-crystalline polyesters and the like.

Examples of elastomers that can be used in the resin compositions of the present invention include diene elastomers and hydrogenated substances thereof such as a polybutadiene, a styrene/butadiene copolymer, an acrylonitrile/butadiene copolymer, an acrylonitrile/styrene/butadiene copolymer, a methyl methacryl ate/ styrene/butadiene copolymer, a polyisopulene and a polychloroprene; olefin elastomers such as anethylene/propylene (ethylidene norbornene) rubber, a butyl rubber, an ethylene/vinyl acetate rubber and ethylene/methyl acrylate; an acrylic rubber mainly composed of acrylic esters, silicone elastomers, fluorine elastomers, urethane elastomers, ester elastomers, amido elastomers and the like.

These elastomers are preferably modified by reactive groups such as acid anhydrides, carboxylic acids, epoxy, hydroxyl, amino, alkoxysilyl and isocyanate groups. The content of such reactive groups is suitably from 0. 001 to 30 mole of the whole elastomer, preferably from 0.01 to 20 mole and optimally from 0.05 to 5 mole %.

Various kinds of catalysts may be added to this system in order to promote the reaction of the maleimide 17 copolymer, polyester resin and elastomer.

The dispersibility and compatibility of each component may be improved by blending polyamino compounds such as a diaminodiphenyl ether, a polyepoxy compound; a resorcin glycidyl ether and a diglycidyl phthalic ether; components capable of reacting with a maleimide copolymers, a polyester resin, an elastomer and the like.

In the present invention, the content (weight ratio) of the alkylmaleimide/olefin copolymer, polyester resin and elastomer is suitably from 1-99:99-1:0-40, preferably from 5-95:95-5:5-40, and optimally from 10-75:90-25:1030. When the content of the alkylmaleimide/olefin copolymer is 1% by weight or less, a resin with poor heat resistance and low rigidity may be obtained. on the other hand, if the elastomer content is 40 by weight or more, a resin with low rigidity may result.

To the resin compositions of the present invention may be blended other resins, for example, an acrylic resin, a polystyrene, a vinyl chloride resin, a polyphenylene ether, a polyacetal, a polyamide, a polyester, a polyphenylene sulphide, a polyimide, polycarbonate, a polysulphone and a fluorine resin, and an elastomer such as a diene elastomer, an olefin elastomer, acrylic elastomer, an urethane elastomer, a fluorine elastomer or a silicone elastomer, or a random, block and graft polymer thereof and the like.

The previously mentioned maleimide and olefins can be polymerized in the presence of rubber-like polymers. and the resulting graft polymers may be used.

At the time of use, to the resin compositions of the present invention may be blended inorganic and organic fillers such as various kinds of dye, glass fibres whose surface may be treated, carbon fibres, potassium titanate, asbestos, silicon carbide, ceramic fibres, metal fibres, silicon nitride, barium sulphate, potassium 18 r sulphate, kaolin, clay, pyrophyllite, zeolite, mical talc, ferrite, calcium silicate, calcium carbonate, magnesium carbonate, antimony trioxide, zinc oxide, titanium oxide, iron oxide, glass balloon and aramide fibres; heat stabilisers such as hindered phenol and organic phosphoric esters; ultraviolet light stabilizer of the benzotriazol series or hindered amine series and the like; flame retarders, blowing agents, antistatic agents, various kinds of lubricant and the like. Further, the moulding objects may be plated, coated, printed and the like.

Though not limiting, the methods for preparing the resin compositions of the present invention include, for example, a method in which an N-alkylsubstituted maleimide/olefin copolymer in the form of powder or pellet and other additives are blended, or they are supplied in an extruder without blending and then meltkneaded.

The invention will now be described with reference to the accompanying drawings, in which:

Fig. 1 is a microphotograph (TEM) of an interface of a sample obtained by Example 9 in accordance with the invention; and Fig. 2 is a microphotograph (TEM) of an interface of a sample obtained by Comparative Example 5.

The resin compositions of the present invention will now be illustrated with reference to the following examples, but the invention is not intended to be limited to these examples.

Examples

The molecular weight of the prepared polymers were calculated by converting into those of polystyrenes using GPC (HLC-802A, TOSOH CORPORATION).

The composition of the prepared polymers was mainly determined by elemental analysis and 'H-NMR spectrometry.

19 The weather resistance of the prepared polymers was estimated from changes in physical properties and appearance after irradiation for 200 hours using a Weather meter (Suga Test Apparatus Co., Ltd.).

The heat distortion temperature, flexural stiffness and flexural modulus, and izod impact strength of the prepared polymers were determined according to ASTM D648f ASTM D790 and ASTM D256, respectively.

Comparative Example A Preparation of N-alkyl-substituted maleimide/olefin copolymers.

Resin A-1 Into an autoclave (50 litres) having a stirring machine, nitrogen- introducing tube, thermometer and deaerating tube were placed 2780 g (25 mole) of N-methyl maleimide, 71 g (0.5 mole) of glycidyl methacrylate, 3.2 g (0.02 mole) of 2,21-azobisisobutyronitrile (AIBN) and 35 liters of dioxane. After the mixture was purged with nitrogen several times, 5610 g (100 mole) of isobuthene was added, and then reacted at 60C f or 12 hours.

The reaction contents were poured into ethanol to separate out a polymer. The polymer was dried under reduced pressure at 600C for 24 hours,, with the yield of 4175 g. By subjecting the resulting polymer to elemental analysis and 'N-NMR spectrometry, it was found that the prepared polymer contained the maleimide units of 49.5 mole % and glycidylmethacrylate units of 0.8 mole %. The resulting polymer had a molecular weight (MW) of 213000. Resin A-2 Into the same reactor as used in A-1 were placed 2780 g (25 mole) of N- methyl maleimide, 48 g (0.4 mole) of 4-aminostyrene, 3.2 g (0.02 mole) of 2,21azobisisobutyronitrile (AIBN) and 35 liters of dioxane. After the mixture was purged with nitrogen several times, 5610 g (50 mole) of isobutene was added, and then it was reacted at 6CC for 12 hours.

The reaction contents were poured into ethanol to separate out a polymer. The polymer was dried under reduced pressure at 600C for 24 hours, with the yield of 4182 g. By subjecting the resulting polymer to elemental analysis and 1-NMR spectrometry,, it was found that the prepared polymer contained the maleimide units of 50.0 mole % and 4-aminostyrene units of 1.0 mole %. The 21 resulting polymer had a molecular weight (MW) of 250000.

Resin A-3 An N-cyclohexyl maleimide/glycidyl methacrylate/ isobuthene copolymer was prepared by the same method as in A-1 except that N-cyclohexyl maleimide was used in place of N-methyl maleimide.

The results of the prepared polymer by elemental analysis showed the polymer contained maleimide units of 51 mole % and glycidylmethacrylate units of 0.6 mole %. The resulting polymer had a molecular weight (MW) of 277000.

Resin A-4 An N-methyl maleimide/isobuthene copolymer was prepared by the same method as used in A-1 without glycidyl methacrylate. The prepared polymer had maleimide units of 50 mole % and a molecular weight (MW) of 240000.

Resin B-1 A copolymer consisting of ethylene units of 91.86 mole %, ethyl acrylate units of 7.93 mole % and maleic anhydride units of 0.21 mole Resin B-2 A copolymer consisting of ethylene units of 97.20 mole %, glycidyl methacrylate units of 2.80 mole Resin B-3 An modified polypropylene which is modified by the reaction extrusion technique, and in which 0.4 mole of maleic anhydride units are grafted.

22 Exam,Ples 1-6 and Comparative Example 1 The maleimide/isobuthene copolymers and olefin resins prepared in the Comparative Example A were previously shaken and blended in the form of powder or pellet of the resin compositions shown in Table 1, and then kneaded and extruded using a biaxial extruder (Laboplastomill; Toyo Seiki Co., Ltd.) twice at 260 to 3200C to form pellets. The resulting pellets were injection-molded using an injection molding press (Panajection; Matsushita Electric Industrial Co., Ltd.) at cylinder temperatures of 260 to 3500C and mold temperatures of 100 to 1400C to prepare samples for measuring physical properties. The obtained results are shown in Tables 1 to 4.

Table 1

Maleimide copolymer Olefin resin by weight) by weight) Example 1 A-1 (80) B-1 (20) 2 A-1 (75) B-2 (25) 3 A-1 (85) B-3 (15) 4 A-2 (80) B-1 (20) A-3 (75) B-1 (25) 6 A-4 (80) B-2 (20) Comparative Example 1 A-4 (100) 23 Table 2

Heat Flexural Flexural Izod SamDle distortion Stiffness modulus impact temDerature (ka/cm2 2 strength (kg/cm (C) (kg.cm/cm) Examnle 1 157 1020 38000 32 2 152 920 34000 48 3 15 5 780 33000 18 4 1-95 920 35000 24 180 780 25000 12 6 153 730 31000 8 Comr)arative ' 1 1350 48500 2 158 ExamDle 1 1 -4 Table 3

Coefficient of Molding Dimensional S amrm) e linear thermal shrinkace chanae rate exDansion (X io--icmlcm.c) Example 1 5.0 0.4 0.04 2 5.6 0.5 0.04 3 5.1 0.6 0.05 4 5.2 0.5 0.04 5.7 0. c; 0.05 6 5.2 0.5 0.04 Commaratve 4.8 0.4 0.08 Example 1 1

After immersion in water at 23C for 24 hours.

Table 4

Before irradiation After irradiation flexural Izod impat flexural lzod impact SamDle stiffness strength stiffness strength (ka (ka.cm/cm) 1CM2 (kg-cm/cm) /CM"-) (kg Example 1 1020 32 1100 32 2 920 48 930 49 3 780 is 760 16 4 920 24 920 25 780 12 730 10 6 730 8 730 7 Comparative 1350 2 1380 2 ExamDle 1 ComDarative Examole B Preparation of N-alkyl- subs ti-tuted maleimidelolefin covolymers Resin A-5 Into an autoclave (50 liters) having a stirring machine, nitrogen- introducing tube, thermometer and deaerating tube were placed 1-780 g (25 male) of N-methyl 26 maleimide, 65 g (0.5 male) of 2-hydroxvethyl methacrylate, 3.2 a (0.02 mole) of 2,21-azobisisobutvronitrile (AIBN) and 35 liters of dioxane. After the mixture was purged with nirroaen several times, 5610 g (100 mole) of isobutene was added, and then reacted at 60C for 12 hours.

The reaction contents were poured into ethanol to separate out a polymer. The polymer was dried under -educed nressure at 600C for 14 hours, with the yield of 4130 a..' my subjecting the resulting polymer to elemental analysis and 1 N-NMR spect-rometry, it was found that the prepared polymer contained the maleimide units of 49.5 mole % and glyc- 4dvlmethacrvlate units of 0.8 mole The resulting polymer had a molecular weight (MW) of 232000.

Resin A-6- Into the same reactor s used in A-5 were placed 2780 g (23 mole) of N-methyl maleimide, 49 g (0.5 mole) of maieic anhvdride 3.2 a (0.02 male) of 2,21 azobisisobutvronitr-4-le (AIEN) and 35 liters of dioxane.

After the mixture was purged with nitrogen several times, 5610 a (50 male) of isobutene was added, and then reacted at 600C for 12 hours.

The reaction contents were poured into ethanal to semarare out a polymer. The polymer was dried under reduced pressure at 600C for 24 hours, with the yield of 4182 g. By subjecting the resulting polymer to elemental analysis and 1 N-NMR smectramet--v, it was found that the 27 prepared polymer conralned the maleimide units of 49.0 male % and maleic anhydride units Of 1.0 mole The resulting polymer had a molecular weight (MW) of 250000.

Rosin A-7 An N-cyclohexyl maleimidelmaleic anhydridelisobuthene copolymer was prepared by the same method as used in A-6 except that N-cyclohexyl malelmide was used in place of N-imethy! maleimide.

The result-3 of th.e mrepared polymer by elemental analysit showed '#--be polymer -contained maleimide units of 51 mole % and maleic anhvdride units of 1.0 mole %. The resulting polymer had a molecular weight (MW) of 197000.

Resin A-8 An N-methv1 maleimidel isobutene copolymer was prepared by the same method as used in A-5 without 2hydroxyethyl methacrylate. The prepared polymer had maleimide units of 550 mole % and a molecular weight (MW) of 240000.

Modified elastcmers Resin B-4 An acr,;lcnit--ile/buthadiene/glycidvI metha=lane copolymer was prepared by the publicly known emulsion colvmer--zarion. The resulting copolymer consisted of acrvlonlt---4.1e of 35 mole %, butadiene of 62 mole %, and glycIdyl merhac--vlate of 3 mole %, with Moonev viscositv of 44. Resin B-5 There as used a commercial available -8 acrylonitrile/butadiene rubber (Japan Synthetic Lubber Co., Ltd.), with Mooney viscosity of 45.

Resin B-6 A modified copolymer consisting of ethyl acrylate of 60 mole %, butyl acrylate of 38 mole %, and glycidyl methacrylate of 2 mole % was prepared by the publicly known suspension polymerization.

Resin B-7 A copolymer consisting of ethyl acrylate of 60 mole %, and butyl acrylate of 40 mole was prepared by the publicly known suspension polymerization.

Resin B-8 A modified elastomer was prepared using an ethylene/ propylene/ethylidenenorbornene elastomer having 1.5 mole % of maleic anhydride graft-polymerized by the reaction extrusion method.

Resin B-9 There was used a commercially available ethylene/ propylene rubber (Japan Synthetic Lubber Co., Ltd.), with Mooney viscosity of 42.

Examples 7-11 and Comparative Examples 2-5 The maleimide copolymers and modified elastomers were previously shaken and blended in the form of powder or pellet of the resin compositions shown in Table 5, and then kneaded and extruded using a biaxial extruder (Laboplastomill; Toyo Seiki Co., Ltd.) twice at 260 to 32TC to form pellets. The resulting pellets were injection-molded using an injection molding press 29 (Panajeczion; Marsusn-,Za Industrial cc=any Co., Ltd.) at cylinder temperatures of 260 to 350C and mold temDeratures of 100 to 140C to prepare samples for measurIna nhysica-l mromerties.

The heat distortion temperature, coefficient of linear thermal expansion, flexural stiffness and flexural modulus, and izod impact strength of the prepared samples were determined according to ASTM D648, ASTM D694, ASTM D790 and ASTM D256, resnectivelv. The obtained results are shown in Table 6.

The interface microstructures of the samples obtained by Example 9 and Comparative Example 5 are shown in Fig. 1 and Fig. 2 respectively. From the photographs it was seen that the individual components were more finely dispersed in Example 9 than in Comparative Example 5.

Comparative Examples 2 to 5 possess non-modified elastomers whereas Examples 7 to 11 contain modified elastomers.

Table 5

Male-imide copolymer Elastomer by weight) by weight) Examz)le 7 A-5 (80) B-4 (20) 8 A-5 (75) B-6 (25) 9 A-5 (85) B-8 (15) A-6 (70) B-8 (30) (80) B-6 (20) ComDarative A-8 (ioo) Examnle 2 3 A-8 (80) B-5 (20) 4 A- 8 (75) B-7 (25) A-8 (85) B-9 (15) sooo ppm d-4ami-nod-J-!!itenyl ether was blended.

Table 6

2 Sample fleat Coefficient of F1exural Flexural. Izod distortion linear thermal stiffness modulus impact temperature expansion (kg/cn,2) (kg/cn,2) stregth OC) (X 10-5cm/cm,C) (kg-cm/cm) Example 7 160 5.1 920 35000 8 157 5.2 850 29000 28 9 158 5.0 890 32000 35 156 5.1 820 27000 52 11 178 5.5 780 24000 21 Comparative Example 2 158 4.9 1200 48000 2 3 152 5.3 330 29000 3 4 142 7.o 280 20000 3 148 6.8 460 21000 2 Comparative Example C Preparation of N-alkyl-substituted maleimide/olefin copolymers.

Resin A-9 Into an autoclave (50 liters) having a stirring machine, nitrogen- introducing tube, thermometer and deaerating tube were placed 2780 g (25 mole) of N-methyl maleimide, 3.2 g (0.02 mole) of 2,21azobisisobutyronitrile (AIBN) and 40 liters of dioxane. After the mixture was purged with nitrogen several times, 2805 g (50 mole) of isobutene was added, and then reacted at 600C f or 12 hours.

The reaction contents were poured into ethanol to separate out a lpolymer. The resulting polymer was purified by reprecipitation with dioxane/ethanol, and then dried under reduced pressure at 600C for 24 hours, with the yield of 4030 g. By subjecting the resulting polymer to elemental analysis (C: 64.7% by weight; H: 7.8% by weight; and N: 8.4% by weight), it was found that the prepared polymer contained the maleimide units of 50 mole % and a molecular weight of 223000.

Resin A-10 Into the same autoclave as used in A-9 were placed 2780 g (25 mole) of N- methyl maleimide, 71 g (0.5 mole) of glycidyl methacrylate, 3.2 g (0.02 mole) of 2,21azobisisobutyronitrile (AIBN) and 35 liters of dioxane. After the mixture was purged with nitrogen several times, 5610 g (100 mole) of isobutene was added, 32 and then it was reacted at 600C for 12 hours.

The reaction contents were poured into ethanol to separate out a polymer. The polymer was dried under reduced mressure at 600C for 24 hours, with the yield of 4175 g.

By subjecting the resulting polymer to elemental analysis and 1 N-NMR spectrometz-1, it was found that the prepared polymer contained the maleimide units of 49.5 mole % and glyciddyl met.hacr71ate units of 0.8 mole The res1t-4na polymer had a molecular weight (MW) of 213000. Resin A! 1 Into the same autoclave as used in A-9 were placed 2780 g (25 mole) of N-methyl maleimide, 49 g (0.5 mole) of maleic anhydride, 3.2 g (0.02 mole) of.2,21--- azobisisobutyranitri4-le (A1BN) and 35 liters of dioxane.

After the mixture was purged with nitrogen several times, 5610 g (100 mole) of isobutene was added, and then it was reactea at 6CC for 12 hours.

The reaction contents were poured into ethanol to separate out a polymer. The polymer was dried under reduced pressure at 60C for 24 hours, with the Yield of 4182 g.

BY subjectina the resulting polymer to elemental analysis and the acid anhydride whose groups were methylesterificated to 1 N-NMR spectrometry, it was found that the prepared polymer contained the maleimide units of 49.0 mole % and maleic anhydride units of 1.0 mole %. The 33 resulting polymer had a molecular weight (MW) of 250000.

Resin A-12 An N-cyclohexyl maleimide/glycidyl methacrylate/ isobuthene copolymer was prepared by the same method as used in A-10 except that N-cyclhexyl maleimide was used in place of N-methyl maleimide.

The results of the prepared polymer by elemental analysis and 'N-NMR spectrometry showed the polymer contained maleimide units of 51 mole % glycidyl methacrylate units of 0.6 mole %. The resulting polymer had a molecular weight (MW) of 277000.

Polyamides and elastomers Resin B-10 Nylon 6 (UBE Nylon 1013 B, UBE INDUSTRIES LTD.) Resin B-11 Nylon 66 (UBE Nylon 2020 B, UBE INDUSTRIES LTD.) Resin C-1 A copolymer consisting of ethylene units of 91.86 mole %, ethyl acrylate units of 7.93 mole and maleic anhydride units of 0.21 mole Resin C-2 A modified ethylene/propylene elastomer in which an ethylene/propylene copolymer consisting of ethylene units of 75 mole % and propylene units of 25 mole and maleic anhydride of 1 mole % is graft-polymerized by the reaction extrusion technique.

Resin C-3 A copolymer consisting of ethyl acrylate units 34 1 of 60 mole %, butyl acr.

71ate units of 38 mole %, and glycidvl methacrylate units of 2 mole %. ExamDle 12 The N-methyl maleimide/isobuthene copolymer (A- 9), polvamide resin (3-10) and elastomer (C-3) prepared in the Reference Example 3 were previously shaken and blended in the form of powder or pellet with composition shown in Table 1, and then kneaded and extruded using a biaxial extruder (LaboDlastomill; Tovo Seiki Co., Ltd.) under the atomosDhere of nitrogen twice at 240 to 280C to form pellets. The resulting milk-white pellets were injection molded using an injectlon molding press (Panajection; Matsushita Electric Industrial Co., Ltd.) at injection molding temperatures of 300C and molded at mold te=eratures of 100C to prepare samples for me 9 physical properties. The obtained results are shown in Table 8.

Exammies 13-17 and Comuarative Examnles 6-7 As in Example 12, the resin compositions shown in Table 7 were melt- kneaded at 260 to 350C to form pellets, which were injectlon-molded at cylinder temueratures of 260 to 3500C and mold temperatures of 80 to 140C to prepare samples. These samples were measured for physical properties. The obtained results are shown in Table 8.

3 5 Table 7

Maleimide Amide Elastomer conolvmer resin (% by weight) by weight) by weight) Examule 12 A-9 (32) 3-10 (55) C-3 (10) 13 A-10 (75) B-10 (53) C-1 (15) 14 A-11 (25) B-10 (63) C-2 (12) A-10 (45) B-11 (45) C-2 (25) 16 A-12 (35) B-11 (40) - 17 A-11 (38) B-11 (62) - Conmarative ExamDle 6 B-10 (100) - 7 B-11 (100) - 0 L0 -1 Fable a Ileat Flexural Flexural 1zod impact strength Sample distortion stiffness modulus (kg.cm/cm) temperature (kg/cm2) (k91cm2) (OC) before after irradiation irradiation Example 12 160 1220 38000 25 23 13 156 1020 35000 38 39 14 155 880 33000 22 22 is 157 920 35000 24 21 16 181 780 28000 14 12 17 160 1260 40000 11 12 Comparative Example 6 60 1100 29000 6 - 7 70 1100 29000 3 CamDarative Examole Preparation of N-alkyl-substituted malelmidelolefin copolymers Resin A-! 3 Into an autoclave (30 liters) having a stirring machine, isobuthene-introducing tube. thermometer and deaerating tube were D-laced 1180 g of N-methyl maleinLide, 153 g of 2-hydroxyethyl methacrylate, 8 g of perbutyl neodecanate and 15 1-4ters of a toluenelmethancl-mixed solventy (an weight ratio of 1:1). After the mixture was purged with nitrogen several times, 8.5 liters of liquef ied Isobutene was added, and then reacted at WC for 12 hours.

The particulate polymer obtained from the reaction was separated out by centritugation and- Ari cd under reduced pressure at 60C for 24 hours, with the yield of 1770 g. The resulting polymer was reprecipitated with a chlarofa=lmethanol solvent: then by subjecting the polymer to elemental analysis and 1 N-MR spectrometry, it was found that the prepared polymer contained the maleimide units of 49.5 mole %, 2-hydrcxvethyl methacrylate units of 1. 0 male % and isobuthene units of 49.5 male %. The resulting polymer had a molecular weight (MW) of 265000. Resin A-14 Into the same reactor as used in A-13 were placed 1180 g N- methvlmaleimide, 23 g of maleic anhydride, 8 g of perbutyl neodecanate and 15 liters of a 8 toluene /methanol-mixed solvent (an weight ratio of 1:1).

After the mixture was purged with nitrogen several times, 8.5 1-4ters of liquefied isobutene was added, and then reacted at 600C JEtr 12 hours.

The particulate polymer obtained from the reaction was separated out by centrifugation and dried under reduced pressure at 60C for 24 hours, with the yield of 1750 g. By subjecting the resulting polymer to elemental analysis, and by subjecting the maleic anhydride portiom of the polymer to 1 N-MR spectrometry, it was found that the prepared polymer contained the maleimide units of 49 mole %, maleic anhydride units of 1.0 mole % and lsobuthene units of 50 mole %. The resulting polymer had a molecular weight (MW) of 270000.

Polvester Resins Resin B-12 Polybuthylene terephthalate (UBE Nylon 2020 B, NOVADUR, Mitsubishi Kasel Corp.) Elastomers Resin C-4 A couolymer consisting of ethylene units of 97.20 mole % and glyc-4dyl methaci-71ate units of 2.80 mole %.

Resin C-5 An erhylenelpronviene elastomer consisting of ethylene units of 730. by weight and propylene units of 27% by weight which was modified with 0.5% by weight.

39 ExamDles 13-21 and Co=arative Examtile 8 The maleim de-isobuthene copolymers, polybuthylene terephthalate resins and elastomers shown in Reference Example 4 were previously shaken and blended in the fo= of powder or pellet of the resin compositions (weight ratio) shown in Table 9, and then kneaded and extruded using a biaxial extruder (Laboplastomill; Toyo Se k Cc., Ltd.) twice at 260 to 320C to fo= pellets. The resulting pellets were injection-molded using an injection molding press (Panajection; Matsushita Electric Industrial Co., Ltd.) at cylinder temperatures of 260 to 3500C and mold temDeratures of 100 to 140C to prepare samDles for measuring physical properties. The obtained results are shown in Table 10.

Table 9

Maleimide Amide Elastomer comolvmer resin (% by weight) (% by weight) by weight) Example 18 A-13 (35) B-12 (55) C-4 (10) 19 A-13 (40) B-12 (45) C-4 (15) A-14 (45) B-12 (43) C-5 (12) 21 A-14 (38) 3-12 (45) C-5 (17) CamDarati've ExamDle 8 1 3-12 (90) C-5 (10) Table 10

Heat Flexural Flexural Izod Sample 1 distortion stiffness modulus impact temperature (ka/cm,,-) (kg/cm2) strength (OC) (kg-cm/cm) Example 18 138 1220 35000 24 19 145 960 34000 29 150 1020 33000 20 21 145 880 30000 25 ComDarative 54 680 20000 13 Examz)le 41

Claims (7)

1. A resin comDosition comprising:

a) a resin which co=rises from 40 to 85 mole % of component (I) and f r c= 60 to 1.5mole % of component (I1) b) an olefin resin; the content of a and b as the ratio a/b being from 5/95 to 99/1 by weight; component 1 having the general formula:

-HC-CH- 0 = C / C = 0 (1) N R, wherein R, represents a C,.-,, alkyl group or a C3-12 cycloalkyl group; and comDonent 11 has the general formula: R3 1 -CH-C 1 1 R2 R, (I1) wherein R2 represents a hydrogen atom or a C,-, alkyl group, and each of R. and R. independently represents a C,8 alkyl group.

2. A resin comDosition comprising: a) a resin which comprises from 40 to 85 mole of component (I) and from 60 to 15mole % of component (I1) as defined in claim 1; and (b) a modified elastomer; the ratio a/b being from 5/95 to 99/1 by weight.

3. A resin c=osition comprising: a) from 1 to 99% by weight of a resin which comprises from 40 to 85 male % of component (I) and from -0 to 15mole % of commonent (I1) as defined in claim 1; 0 - b) from 1 "-,,o 99% by weight of a polyamide resin; 42 t and c) from 0 to 40% by weight of an elastomer.

4. A resin comDosition comprising:

a) from 1 to 99% by weight of a resin which comprises from 40 to 85- male % of component (I) and from 60 to 15mole -'. of component (I1) as defined in claim 1; b) from 1 to 99% by weight of a polyester resin; and c) from 0 to 40% by weight of an elastomer.

5. A heat-resistant resin composition as claimed in any of claims 1 to 4 wherein R, is a methyl, ethyl, isopropyl or cyclohexyl group.

6. A resin composition according to any one of Claims 1 to 4 wherein the modified elastomer is an elastomer having a reactive group as defined in Claim 5.

is

7. A resin composition according to any preceding claim wherein in resin (a) the weight-average molecular weight (converted into that of polystyrene) is from 1 X 103 to 5 X 106.

4L

6. A resin composition as claimed in any of claims 1 to 5 wherein R, represents a hydrogen atom and each of R., and R, is a methyl group.

7. A resin comDosition as claimed in claim 1 wherein the olefin resin is a polyethylene, a polypropylene, a poly-4 -methyl -1-pentene or a modified derivative thereof.

8. A resin composition as claimed in claim 2 wherein the modified elastomer is a modified substance such as a diene elastomer or a hydrogenated elastomer thereof, an olefin elastcmer, an acrylic elastomer, a silicone elastomer, a fluorine elastomer, a urethane elastcmer, an ester elaszcmer and/or an amide elastomer.

9. A resin composition as claimed in claim 3 wherein the polyamide resin is nylon 6, nylon 66, nylon 610, nylon 612, nylon 11, nylon 12 and/or nylon 46.

43 10. A resin composition as claimed in claim 4 wherein the polyester resin is a polybutylene terephthalate, a polvethylene terephthalate, a polyarylate and/or a liquid-crystalline polyester.

11. A resin c=osition according to any of claims 1 to 4, wherein the resin a) is modified by possessing or introducing one or more reactive groups.

12. A resin comDosition according to claim 11 wherein the or each reactive grcuD is a carboxylic acid, a derivative thereof, an acid anhvdride, hydroxyl, amino, thiol, epoxy, alkoxyl silyl and/or isocyanate group.

13. A resin comDosition according to claim 8 wherein the modified substance is an elastomer having a reactive group as defined in claim 12.

14. A resin comDosition according to claim 3 or 4, wherein the elastomer has a reactive group as defined in claim 12.

15. A resin composition according to any preceding claim wherein in resin (a) the weight-average molecular weight (converted into that of polystyrene) is from 1 X 103 to 5 X 106.

44 Amendments to the claims have been filed as follows is 1. A resin composition comprising:

a) a resin which comprises from 40 to 85 mole -0. of component (I) and from 60 to 15 mole 0-. of component (II) component I having the general formula:

_HC-CH- 0 = C C = 0 N ke.1 (1) wherein R1 represents a C,-,, alkyl group or a C3-12 cycloalkyl group; and component II Has the general formula:

R3 R2 R4 (II) wherein R2 represents a hydrogen atom or a C,, alkyl group, and each of R3 and R4 independently represents a C,-, alkyl group, and b) a modif ied elastomer which is a diene elastomer or a hydrogenated elastomer thereof, an olef in elastomer, an acrylic elastomer, a silicone elastomer, a fluorine elastomer, a urethane elastomer, an ester elastomer or an amide elastomer, or a mixture thereof, or an olefin resin which is a polyethylene, a polypropylene, a poly-4methyl-l-pentene or a modified derivative thereof, the ratio a/b being from 5/95 to 99/1 by weight.

2. A heat-resistant resin composition as claimed in Claim 1 wherein R, is a methyl, ethyl, isopropyl or cyclohexyl group.

3. A resin composition as claimed in Claim 1 or Claim 2 wherein R2 represents a hydrogen atom and each of F ts R3 and R, is a methyl group.

4. A resin composition according to any of Claims 1 to 3, wherein the resin a) is modified by possessing or introducing one or more reactive groups.

1 5. A resin composition according to Claim 4 wherein the or each reactive group is a carboxylic acid, a derivative thereof, an acid anhydride, hydroxyl, amino, thiol, epoxy, alkoxyl silyl and/or isocyanate group.