US4904758A
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Low-melting polyimide copolymer and method for preparing the same
Assignee: JNC Corp
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Filing: 1989-01-05
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Granted: 1990-02-27
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Expires: 2009-01-05
Abstract
Abstract The present invention is connected with a low-melting polyimide copolymer containing 30 to 90 mole % of an imide repeating unit represented by the following formula (I) and 10 to 70 mole % of an imide repeating unit represented by the following formula (II), and having a logarithmic viscosity number of 0.1 to 4 dl/g: ##STR1## wherein R 1 is at least one of ##STR2## Furthermore, the present invention is connected with a method of preparing the low-melting polyimide copolymer. Since having a melting point of about 300° to about 400° C., the polyimide copolymer of the present invention has heat resistance and enables melt-moldings such as extrusion and injection molding.
Inventors
- 👤 Kouichi Kunimune
- 👤 Hirotoshi Maeda
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-01 20:58
CPC Classifications
C; C08; C08G; C08G73/00; C08G73/06; C08G73/10; C08G73/1042; C08G73/1067; C08G73/1071
Claims Analysis
Total Claims: 9
Claim 1
Independent Claim
123 words
A low-melting polyimide copolymer containing 30 to 90 mole % of the following imide repeating unit (I), containing 10 to 70 mole % of the following imide repeating unit (II), containing or not containing the following imide repeating unit (III), and having a logarithmic viscosity number of 0.1 to 5 dl/g when measured in concentrated sulfuric acid at a temperature of 30°±0.01° C. at a concentration of 0.5 g/dl: ##STR20## wherein R 1 is at least one of ##STR21## R 4 is at least one of ##STR22## R 5 is a carbon cyclic aromatic group having 6 to 50 carbon atoms, but when R 4 is ##STR23## R 5 is neither ##STR24## and when R 5 is ##STR25## R 4 is not ##STR26##
Claim 2
Dependent Claim
123 words
A low-melting polyimide copolymer containing 30 to 90 mole % of the following imide repeating unit (I), containing 10 to 70 mole % of the following imide repeating unit (II), containing or not containing the following imide repeating unit (III), and having a logarithmic viscosity number of 0.1 to 5 dl/g when measured in concentrated sulfuric acid at a temperature of 30°±0.01° C. at a concentration of 0.5 g/dl: ##STR20## wherein R 1 is at least one of ##STR21## R 4 is at least one of ##STR22## R 5 is a carbon cyclic aromatic group having 6 to 50 carbon atoms, but when R 4 is ##STR23## R 5 is neither ##STR24## and when R 5 is ##STR25## R 4 is not ##STR26##
Claim 3
Dependent Claim
30 words
A low-melting polyimide copolymer according to claim 1 wherein the copolymer has a melting point in the range of 300° to 400° C. when measured by a differential scanning calorimeter.
Claim 4
Independent Claim
416 words
A method for preparing a low-melting polyimide copolymer containing 30 to 90 mole % of the following imide repeating unit (I), containing 10 to 70 mole % of the following imide repeating unit (II), containing or not containing the following imide repeating unit (III), and having a logarithmic viscosity number of 0.1 to 5 dl/g when measured in concentrated sulfuric acid at a temperature of 30°±0.01° C. at a concentration of 0.5 g/dl, the aforesaid method being characterized by comprising the steps of feeding raw materials at one time or dividedly to a reactor; reacting diacid anhydrides of A 1 mole of a compound represented by the following formula (IV) and A 2 mole of a compound represented by the following formula (V) with diamines of B 1 mole of a compound represented by the following formula (VI), B 2 mole of a compound represented by the following formula (VII) and B 3 mole of a compound represented by the following formula (VIII) in compliance with relations of formulae (IX), (X), (XI) and (XII) regarding A 1 , A 2 , B 1 , B 2 and B 3 in the presence of a solvent at a temperature of 0° to 200° C. under conditions where the acid anhydride represented by th formula (IV) which accounts for at least 30 mole % of the whole diacid anhydride is reacted with the diamine represented by the formula (VI) which accounts for at least 30 mole % of the whole diamine and under conditions where the diacid anhydride represented by the formula (IV) which accounts for at least 10 mole % of the whole diacid anhydride is reacted with the diamine represented by the formula (VII) which accounts for at least 10 mole % of the whole diamine, in order to form a polyimide precursor; and heating the precursor at 100° to 400° C. or adding a known imide formation accelerator thereto and converting the precursor into the imide at a relatively low temperature of 10° to 100° C.: ##STR27## wherein R 1 is at least one of ##STR28## R 2 is at least one of ##STR29## R 3 is a carbon cyclic aromatic group having 6 to 50 carbon atoms except ##STR30## R 4 is at least one of ##STR31## and R 5 is a carbon cyclic aromatic group having 6 to 50 carbon atoms, but when R 4 is ##STR32## R 5 is neither ##STR33## and when R 5 is ##STR34## R 4 is not ##STR35##
Claim 5
Independent Claim
416 words
A method for preparing a low-melting polyimide copolymer containing 30 to 90 mole % of the following imide repeating unit (I), containing 10 to 70 mole % of the following imide repeating unit (II), containing or not containing the following imide repeating unit (III), and having a logarithmic viscosity number of 0.1 to 5 dl/g when measured in concentrated sulfuric acid at a temperature of 30°±0.01° C. at a concentration of 0.5 g/dl, the aforesaid method being characterized by comprising the steps of feeding raw materials at one time or dividedly to a reactor; reacting diacid anhydrides of A 1 mole of a compound represented by the following formula (IV) and A 2 mole of a compound represented by the following formula (V) with diamines of B 1 mole of a compound represented by the following formula (VI), B 2 mole of a compound represented by the following formula (VII) and B 3 mole of a compound represented by the following formula (VIII) in compliance with relations of formulae (IX), (X), (XI) and (XII) regarding A 1 , A 2 , B 1 , B 2 and B 3 in the presence of a solvent at a temperature of 0° to 200° C. under conditions where the acid anhydride represented by th formula (IV) which accounts for at least 30 mole % of the whole diacid anhydride is reacted with the diamine represented by the formula (VI) which accounts for at least 30 mole % of the whole diamine and under conditions where the diacid anhydride represented by the formula (IV) which accounts for at least 10 mole % of the whole diacid anhydride is reacted with the diamine represented by the formula (VII) which accounts for at least 10 mole % of the whole diamine, in order to form a polyimide precursor; and heating the precursor at 100° to 400° C. or adding a known imide formation accelerator thereto and converting the precursor into the imide at a relatively low temperature of 10° to 100° C.: ##STR27## wherein R 1 is at least one of ##STR28## R 2 is at least one of ##STR29## R 3 is a carbon cyclic aromatic group having 6 to 50 carbon atoms except ##STR30## R 4 is at least one of ##STR31## and R 5 is a carbon cyclic aromatic group having 6 to 50 carbon atoms, but when R 4 is ##STR32## R 5 is neither ##STR33## and when R 5 is ##STR34## R 4 is not ##STR35##
Claim 6
Dependent Claim
49 words
A method for preparing a low-melting polyimide copolymer according to claim 3 wherein the tetracarboxylic acid dianhydride represented by the general formula (V) is at least one selected from the group consisting of pyromellitic acid dianhydride, 3,3',4,4'-benzophenonetetracarboxylic acid dianhydride, 2,3,3',4'-benzophenonetetracarboxylic acid dianhydride, bis(3,4-dicarboxyphenyl) ether dianhydride and bis(3,4-dicarboxyphenyl) sulfone dianhydride.
Claim 7
Dependent Claim
35 words
A method for preparing a low-melting polyimide copolymer according to claim 3 wherein the diamine represented by the general formula (VII) is at least one selected from the group consisting of methaphenylenediamine and 3,4'-diaminodiphenyl ether.
Claim 8
Dependent Claim
56 words
A method for preparing a low-melting polyimide copolymer according to claim 3 wherein the diamine represented by the general formula (VIII) is at least one selected from the group consisting of 4,4'-diaminodiphenyl ether, 4,4'-diaminodiphenylmethane, 3,3'-diaminodiphenyl sulfone, 4,4'-diaminodiphenyl sulfone, 4,4'-diaminodiphenyl sulfide, 4,4'-di(meta-aminophenoxy)diphenyl sulfone, 4,4'-di(para-aminophenoxy)diphenyl sulfone, para-phenylenediamine, benzidine, 2,2'-diaminobenzophenone, 4,4'-diaminobenzophenone, 2,2-bis[4-(4-aminophenoxy)phenyl]propane, 1,4-bis(4-aminophenoxy)benzene, 1,3-bis(4-aminophenoxy)benzene, 1,3-bis(3-aminophenoxy)benzene, 1,5-diaminonaphthalene, 1,8-diaminonaphthalene and 2,2-bis[4-(4-aminophenoxy)phenyl]hexafluoropropane.
Claim 9
Dependent Claim
49 words
A method for preparing a low-melting polyimide copolymer according to claim 3 wherein a solvent, in which the above-mentioned raw material compounds are dissolved and reacted, is at least one selected from the group consisting of N-methyl-2-pyrrolidone, dimethylacetamide, dimethylformamide, dimethyl sulfoxide, tetramethylurea, pyridine, dimethyl sulfone, hexamethylphosphoneamide, methylformamide and N-acetyl-2-pyrrolidone.
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USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 1993-02-26 | 1993-08-28 | 1994-02-27 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1997-02-26 | 1997-08-28 | 1998-02-27 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 2001-02-26 | 2001-08-28 | 2002-02-27 | $7700.00 | Window Closed / Lapsed |