Polyimide and preparation process of same

Claim 2

A polyimide comprising a requisite structural unit having one or more recurring structural units of the formula ( 1): ##STR85## wherein X 1 is a direct bond or a divalent radical selected from the group consisting of --O--, --CO-- and --C(CH 3 )-- and two X 1 are the same or different from each other, m is an integer of 1˜6, n is individually 0 or an integer of 1˜4, R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and Ar is a divalent radical selected from the group consisting of ##STR86## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and --C(CH 3 ) 2 --, m is an integer of 1˜6, and p is individually 0 or an integer of 1˜4, or an integer of 1˜4 when n is 0 in the formula (1).

Claim 3

A capped polyimide comprising a requisite structural unit having one or more recurring structural units of the formula (1): ##STR87## wherein X 1 is a direct bond or a divalent radical selected from the group consisting of --O--, --CO-- and --C(CH 3 )-- and two X 1 are the same or different from each other, m is an integer of 1˜6, n is individually 0 or an integer of 1˜4, R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and Ar is a divalent radical selected from the group consisting of ##STR88## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and --C(CH 3 ) 2 --, m is an integer of 1˜6, and p is individually 0 or an integer of 1˜4, or an integer of 1˜4 when n is 0 in the formula (1), and having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for amine and dicarboxylic anhydride.

Claim 4

A capped polyimide comprising a requisite structural unit having one or more recurring structural units of the formula (1): ##STR87## wherein X 1 is a direct bond or a divalent radical selected from the group consisting of --O--, --CO-- and --C(CH 3 )-- and two X 1 are the same or different from each other, m is an integer of 1˜6, n is individually 0 or an integer of 1˜4, R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and Ar is a divalent radical selected from the group consisting of ##STR88## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and --C(CH 3 ) 2 --, m is an integer of 1˜6, and p is individually 0 or an integer of 1˜4, or an integer of 1˜4 when n is 0 in the formula (1), and having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for amine and dicarboxylic anhydride.

Claim 5

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (11): ##STR89## wherein X 1 is a direct bond or a divalent radical selected from the group consisting o --O--, --S--, --CO-- and --C(CH 3 ) 2 --, and n and p or 0 or an integer of 1˜4 and are not simultaneously 0, and R is a tetravalent radical having 2-27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 6

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (11): ##STR89## wherein X 1 is a direct bond or a divalent radical selected from the group consisting o --O--, --S--, --CO-- and --C(CH 3 ) 2 --, and n and p or 0 or an integer of 1˜4 and are not simultaneously 0, and R is a tetravalent radical having 2-27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 7

A preparation process of polyimide comprising a requisite structural unit having one or more recurring structural units of the formula (1): ##STR90## wherein X 1 is a direct bond or a divalent radical selected from the group consisting of --O--, --CO-- and --C(H 3 ) 2 --, two X 1 may be same or different, m is an integer of 1˜6, n is 0 or an integer of 1˜4, and Ar is a divalent radical selected from the group consisting of ##STR91## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and ----C(CH 3 ) 2 , m is an integer of 1˜6, and p individually 0 or an integer of 1˜4, and an integer of 1˜4 when n=0 in the formula (1), R is tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, which comprises reacting an aromatic diamine having one or more principal ingredients of the formula (13): ##STR92## wherein X 1 , Ar, m and n are the same as above, with one or more tetracarboxylic dianhydride principally represented by the formula (14): ##STR93## wherein R are the same as above, and thermally or chemically imidizing the resulting polyamic acid.

Claim 8

A preparation process of polyimide comprising a requisite structural unit having one or more recurring structural units of the formula (1): ##STR90## wherein X 1 is a direct bond or a divalent radical selected from the group consisting of --O--, --CO-- and --C(H 3 ) 2 --, two X 1 may be same or different, m is an integer of 1˜6, n is 0 or an integer of 1˜4, and Ar is a divalent radical selected from the group consisting of ##STR91## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and ----C(CH 3 ) 2 , m is an integer of 1˜6, and p individually 0 or an integer of 1˜4, and an integer of 1˜4 when n=0 in the formula (1), R is tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, which comprises reacting an aromatic diamine having one or more principal ingredients of the formula (13): ##STR92## wherein X 1 , Ar, m and n are the same as above, with one or more tetracarboxylic dianhydride principally represented by the formula (14): ##STR93## wherein R are the same as above, and thermally or chemically imidizing the resulting polyamic acid.

Claim 9

A preparation process of capped aromatic polyimide comprising a requisite structural unit having one or more recurring structural units of the formula (1): ##STR94## wherein X is a direct bond or a divalent radical selected from the group consisting of --O--, --CO-- and --C(CH 3 ) 2 --, two X 1 are the same or different, m is an integer of 1˜6, n is ) or an integer of 1˜4, and Ar is a divalent radical selected from the group consisting of ##STR95## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and --C(CH 3 ) 2 --, m is an integer of 1˜6, and p individually 0 or an integer of 1˜4, and an integer of 1˜4 when n=0 in the formula (1), R is tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for amine and dicarboxylic anhydride, comprising reacting aromatic diamine having one or more principal ingredients of the formula (13): ##STR96## wherein X 1 , Ar, m, and n are the same as above, with one or more tetracarboxylic dianhydride principally represented by the formula (14) ##STR97## wherein R is the same as above, in the presence of aromatic dicarboxylic anhydride of the formula (15): ##STR98## wherein Z is a divalent radical having 6˜15 carbon atoms and being selected from the group consisting of a monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and/or aromatic monoamine of the formula (16) Z.sub.1 --NH.sub.2 ( 16) wherein Z 1 is a monovalent radical having 6˜15 carbon atoms and being selected from the group consisting of a monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and thermally or chemically imidizing the resulting polyamic acid.

Claim 10

A preparation process of capped aromatic polyimide comprising a requisite structural unit having one or more recurring structural units of the formula (1): ##STR94## wherein X is a direct bond or a divalent radical selected from the group consisting of --O--, --CO-- and --C(CH 3 ) 2 --, two X 1 are the same or different, m is an integer of 1˜6, n is ) or an integer of 1˜4, and Ar is a divalent radical selected from the group consisting of ##STR95## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and --C(CH 3 ) 2 --, m is an integer of 1˜6, and p individually 0 or an integer of 1˜4, and an integer of 1˜4 when n=0 in the formula (1), R is tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for amine and dicarboxylic anhydride, comprising reacting aromatic diamine having one or more principal ingredients of the formula (13): ##STR96## wherein X 1 , Ar, m, and n are the same as above, with one or more tetracarboxylic dianhydride principally represented by the formula (14) ##STR97## wherein R is the same as above, in the presence of aromatic dicarboxylic anhydride of the formula (15): ##STR98## wherein Z is a divalent radical having 6˜15 carbon atoms and being selected from the group consisting of a monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and/or aromatic monoamine of the formula (16) Z.sub.1 --NH.sub.2 ( 16) wherein Z 1 is a monovalent radical having 6˜15 carbon atoms and being selected from the group consisting of a monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member, and thermally or chemically imidizing the resulting polyamic acid.

Claim 11

The preparation process of claim 4 or claim 5 wherein the aromatic diamine has the formula (17): ##STR99## wherein m is an integer of 1˜6, n is 0 or an integer of 1˜4, and Ar is a divalent radical selected from the group consisting of ##STR100## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and --C(CH 3 ) 2 --, m is an integer of 1˜6, and p is 0 or an integer of 1˜4, and is an integer of 1˜4 when n is 0 in the formula (17).

Claim 12

The preparation process of claim 4 or claim 5 wherein the aromatic diamine has the formula (21): ##STR101## wherein X 2 is a direct bond or a divalent radical selected from the group consisting of --O--, --S--, --CO-- and --C(CH 3 ) 2 --, and n and p are individually 0 or an integer of 1˜4 and are not simultaneously 0.

Claim 13

The polyimide of claim 1 or claim 2 wherein the polyimide having the recurring structural units of the formula (1) is derived from the polyamic acid precursor having an inherent viscosity of 0.01˜3.0 dl/g at a concentration of 0.5 g/dl in a dimethylacetamide solution at 35° C.

Claim 14

A polyimide of claim 1 or claim 2 wherein the polyimide having reccuring structural units of the formula (1) has an inherent viscosity of 0.01˜3.0 dl/g at 35° C. at a concentration of 0.5 g/dl in a solvent mixture composed of 9 parts by weight p-chlorophenol and 1 part by weight of phenol.

Claim 15

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (2): ##STR102## wherein n and p are 0 or an integer of 1˜4, and are not simultaneously 0, and R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 16

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (2): ##STR102## wherein n and p are 0 or an integer of 1˜4, and are not simultaneously 0, and R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 17

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (3): ##STR103## wherein n is an integer of 1˜4 and R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, mono aromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 18

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (3): ##STR103## wherein n is an integer of 1˜4 and R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, mono aromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 19

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (4): ##STR104## wherein n is an integer of 1˜4 and R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 20

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (4): ##STR104## wherein n is an integer of 1˜4 and R is a tetravalent radical having 2˜27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 21

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units selected from the group consisting of the formulas (5), (6), (7), (8), (9) and (10): ##STR105## wherein R is a tetravalent radical having 2-27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 22

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units selected from the group consisting of the formulas (5), (6), (7), (8), (9) and (10): ##STR105## wherein R is a tetravalent radical having 2-27 carbon atoms and being selected from the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 23

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (12): ##STR106## wherein R is a tetravalent radical having 2˜27 carbon atoms and being selected form the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 24

An aromatic polyimide or a capped aromatic polyimide having at the polymer chain end thereof an aromatic ring which is essentially unsubstituted or substituted with a radical having no reactivity for dicarboxylic anhydride, comprising a requisite structural unit having one or more recurring structural units of the formula (12): ##STR106## wherein R is a tetravalent radical having 2˜27 carbon atoms and being selected form the group consisting of an aliphatic radical, alicyclic radical, monoaromatic radical, condensed polyaromatic radical and noncondensed aromatic radical connected to each other with a direct bond or a bridge member.

Claim 25

The preparation process of claim 4 or claim 5 wherein the aromatic diamine has the formula (18): ##STR107## wherein n and p are 0 or an integer of 1, and are not simultaneously 0.

Claim 26

The preparation process of claim 4 or claim 5 wherein the aromatic diamine has the formula (19): ##STR108## wherein n is an integer of 1˜4.

Claim 27

The preparation process of claim 4 or claim 5 wherein the aromatic diamine has the formula (20): ##STR109## wherein p is an integer of 1˜4.

Claim 28

The preparation process of claim 4 or claim 5 wherein the aromatic diamine is one or more compounds selected from the group consisting of 1,3-bis(3-aminophenoxy)-4-trifluoromethylbenzene, 1,3-bis(3-aminophenoxy)-5-trifluoromethylbenzene, 1,3-bis(3-amino-5-trifluoromethylphenoxy)benzene, 1,4-bis(3-amino-5-trifluoromethylphenoxy)benzene and 1,3-bis(3-amino-5-trifluoromethylphenoxy)-4-trifluoromethylbenzene.

Claim 29

The preparation process of claim 4 or claim 5 wherein the aromatic diamine has the formula (22): ##STR110##

Claim 30

The preparation process of claim 4 or claim 5 wherein the aromatic diamine is 4,4-bis(3-amino-5-fluoromethylphenoxy)biphenyl.

Claim 31

The preparation process of claim 5 wherein the aromatic dicarboxylic anhydride is phthalic anhydride.

Claim 32

The preparation process of claim 5 wherein the aromatic monoamine is aniline.

Claim 33

The preparation process of claim 5 wherein the amount of the aromatic dicarboxylic anhydride is 0.001˜1.0 mol per mol of the aromatic diamine.

Claim 34

The preparation process of claim 23 wherein the amount of phthalic anhydride is 0.001˜1.0 mol per mol of the aromatic diamine.

Claim 35

The preparation process of claim 5 wherein the amount of the aromatic monoamine is 0.001˜1.0 mol per mol of the tetracarboxylic dianhydride.

Claim 36

The preparation process of claim 25 wherein the amount of aniline is 0.001˜1.0 mol per mol of the tetracarboxylic dianhydride.

Claim 37

A composition comprising polyimide in one of claims 1, 2, 3, 10, 11, 12, 13, and 14.

Claim 38

A polyimide film comprising polyimide in one of claims 1, 2, 3, 10, 11, 12, 13, and 14.