EP0200204A2 — Melt-fusible copolyimides

Claim 1

Independent Claim 286 words

A melt-fusible copolyimide consisting essentially of two types of repeating units ano where Q is at least one divalent organic radical represented by the following formula (3): where G is selected from the group consisting of isopropylidene, O, S, CH 2 , SO 2 , and CO; and n is 0 or 1; neither one of the terminal bonds being in the ortho position to any other covalent bond; and X is at least one divalent organic radical represented by the following formula (4): where G' is selected from the group consisting of O, S, S0 2 , and CO; each of m, p, and q individually is 0 or 1; but, when any one of m, p, and q is not 0, then at least two of m, p, ana q are 1; Z is hydrogen, phenyl, or one of but when m=p=q=O, Z is not hydrogen ana is not in the ortho position with respect to both terminal bonas, and the two terminal bonds are not ortho to each other; further provided that any aromatic ring other than the aromatic rings carrying the pendant covalent bonds may be substituted by chlorine, so long as the number of chlorine atoms in the molecule does not exceed 4, and the maximum number of chlorine atoms per aromatic ring is 2; the mole proportion, t, of the repeating units of the type represented by formula (1) being about 10-90%, and the mole proportion, u, of the repeating units represented by formula (2) being about 90-10%, the minimum value of u being such that u = 100-10(m+p)-15(q+n)-0.3(z-1) mole %, where z is the formula weight of Z; u always being calculateo for X having the smallest formula weight.

Claim 2

Dependent Claim 286 words

A melt-fusible copolyimide consisting essentially of two types of repeating units ano where Q is at least one divalent organic radical represented by the following formula (3): where G is selected from the group consisting of isopropylidene, O, S, CH 2 , SO 2 , and CO; and n is 0 or 1; neither one of the terminal bonds being in the ortho position to any other covalent bond; and X is at least one divalent organic radical represented by the following formula (4): where G' is selected from the group consisting of O, S, S0 2 , and CO; each of m, p, and q individually is 0 or 1; but, when any one of m, p, and q is not 0, then at least two of m, p, ana q are 1; Z is hydrogen, phenyl, or one of but when m=p=q=O, Z is not hydrogen ana is not in the ortho position with respect to both terminal bonas, and the two terminal bonds are not ortho to each other; further provided that any aromatic ring other than the aromatic rings carrying the pendant covalent bonds may be substituted by chlorine, so long as the number of chlorine atoms in the molecule does not exceed 4, and the maximum number of chlorine atoms per aromatic ring is 2; the mole proportion, t, of the repeating units of the type represented by formula (1) being about 10-90%, and the mole proportion, u, of the repeating units represented by formula (2) being about 90-10%, the minimum value of u being such that u = 100-10(m+p)-15(q+n)-0.3(z-1) mole %, where z is the formula weight of Z; u always being calculateo for X having the smallest formula weight.

Claim 3

Dependent Claim 36 words

The copolyimide of Claim 1 in which Q is the divalent radical remaining after removal of the amine groups from bis(4-aminophenyl)methane, and X is the divalent radical remaining after removal of the amine groups from 2,2-bis(4-aminophenoxyphenyl)-propane.

Claim 4

Dependent Claim 37 words

The copolyimide of Claim 1 in which Q is the divalent radical remaining after removal of the amine groups from 4,4'-diaminodiphenyl ether, ana X is the divalent radical remaining after removal of the amine groups from l,3-bis(3-aminophenoxy)benzene.

Claim 5

Dependent Claim 34 words

A polyimide of Claim 1 wherein the divalent radical Q is obtained by removing the amine groups from at least one of the following diamines: 4,4'-diaminodiphenyl ether; 4,4'-aiaminodiphenylmethane; 1,3-diaminobenzene; 1,4-diaminobenzene; 1,4-diaminodiphenylsulfone; and 1,4-diaminodiphenyl sulfide.

Claim 6

Dependent Claim 31 words

A polyimide of Claim 1 wherein the divalent radical X is obtained by removing the amine groups from at least one of the following diamines: l,3-bis(3-aminophenoxybenzene); 2,2-bis(4-aminophenoxyphenyl)propane; 2,2-bis(4-aminophenoxy-3,5-dichlorophenyl)-propane; 2-(2,4-diaminophenoxy)biphenyl; and 2-phenyl-l,4-bis(4-aminophenoxy)-benzene.

Claim 7

Dependent Claim 48 words

A prepreg consisting essentially of a fibrous substrate impregnated with a concentrated solution of a polyimide of Claim 1 in an appropriate solvent, the amount of volatiles being about 25 weight percent or less, and the volume proportion of fibers, on volatiles-free basis, being up to about 70%.

Claim 8

Dependent Claim 14 words

A prepreg of Claim 6 wherein the volatiles content is about 10-20 weight percent.

Claim 9

Dependent Claim 17 words

A prepreg of Claim 6 wherein the volume proportion of fibers, on volatiles-free basis is about 40-65%.

Claim 10

Dependent Claim 18 words

A cured prepreg obtained by impregnating a fibrous substrate with an end-capped nonstoichiometric molten polyimide of Claim 1.

Claim 11

Dependent Claim 47 words

A precursor solution for making a polyimide of Claim 1, consisting essentially of pyromellitic anhydride, a diamine H 2 NQNH 2 , and diamine H 2 NXNH 2 in an appropriate solvent and in appropriate stoichiometric proportions to form after complete reaction a polyimide of Claim 1.

Claim 12

Dependent Claim 73 words

A precursor solution for making an end capped polyimide of Claim 1, consisting essentially of pyromellitic anhydride, a diamine H 2 NQNH 2 , a diamine H 2 NXNH 2 , and an end-capping agent in an appropriate solvent and in such proportions that there is present in the solution an excess of either a diamine or pyromellitic dianhydride, and the amount of the end-capping agent is about stoichiometrically equivalent to that excess.

Claim 13

Dependent Claim 18 words

A filled polyimide composition consisting essentially of a polyimiae of Claim 1 and a fibrous or particulate filler.

Claim 14

Dependent Claim 23 words

A filled polyimide composition of Claim 12, wherein the filler is fibrous and its content in the composition is about 5-70 volume percent.

Claim 15

Dependent Claim 20 words

A filled polyimide composition of Claim 12, wherein the filler is particulate and its content is about 5-50 volume percent.

Claim 16

Dependent Claim 16 words

A filled polyimide composition of Claim 14, wherein the filler content is about 5-25 volume percent.

Claim 17

Dependent Claim 17 words

A fabricated polyimide article made by extrusion, compression, casting, injection, or drawing a polyimide of Claim 1.

Claim 18

Dependent Claim 19 words

A fabricated filled polyimide article made by compression, extrusion, casting, injection, or drawing a filled polyimide of Claim 12.

Melt-fusible copolyimides

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