US4778872A
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Polyamic acid solution composition and polymide film made therefrom
Assignee: Ube Corp
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Filing: 1985-11-04
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Granted: 1988-10-18
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Expires: 2005-11-04
Abstract
Abstract Disclosed is an aromatic polyamic acid solution composition comprising an aromatic polyamic acid dissolved in an amount of 5 to 40% by weight in an organic polar solvent. The aromatic polyamic acid is prepared by polymerizing substantially equimolar amounts of an aromatic tetracarboxylic acid component comprising 15 to 85 mole % of a biphenyltetracarboxylic acid or its functional derivative and 15 to 85 mole % of a pyromellitic acid or its functional derivative and an aromatic diamine component comprising 30 to 100 mole % of a phenylenediamine and 0 to 70 mole % of a diaminodiphenyl ether. The aromatic polyamic acid solution composition is formed into an aromatic polyimide film having a relatively small thermal expansion coefficient, high mechanical strength and good flexibility.
Inventors
- 👤 Yoshikazu Sasaki
- 👤 Hiroshi Inoue
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-04 16:03
CPC Classifications
C; C08; C08L; C08L79/00; C08L79/04; C08L79/08; C08G; C08G73/00; C08G73/06; C08G73/10; C08G73/1003; C08G73/1007; C08G73/1067; C08G73/1071; H; H05; H05K; H05K1/00; H05K1/02; H05K1/03; H05K1/0313; H05K1/032; H05K1/0346
Claims Analysis
Total Claims: 30
Claim 1
Independent Claim
141 words
An aromatic polyamic acid solution composition comprising an aromatic polyamic acid, which when imidized forms an aromatic polyamide having essentially imide linkages as the linkage of main chain, dissolved in an amount of 5 to 40% by weight in an organic polar solvent, said aromatic polyamic acid being prepared by polymerizing substantially equimolar amounts of: (a) an aromatic tetracarboxylic acid component consisting essentially of, based on the total amount of the aromatic tetracarboxylic acid component, 15 to 85 mole % of a biphenyltetracarboxylic acid or a functional derivative thereof and 15 to 85 mole % of a pyromellitic acid or a functional derivative thereof, and (b) an aromatic diamine component consisting essentially of, based on the total amount of the aromatic diamine component, 30 to 100 mole % of a phenylenediamine and 0 to 70 mole % of a diaminodiphenyl ether.
Claim 2
Dependent Claim
141 words
An aromatic polyamic acid solution composition comprising an aromatic polyamic acid, which when imidized forms an aromatic polyamide having essentially imide linkages as the linkage of main chain, dissolved in an amount of 5 to 40% by weight in an organic polar solvent, said aromatic polyamic acid being prepared by polymerizing substantially equimolar amounts of: (a) an aromatic tetracarboxylic acid component consisting essentially of, based on the total amount of the aromatic tetracarboxylic acid component, 15 to 85 mole % of a biphenyltetracarboxylic acid or a functional derivative thereof and 15 to 85 mole % of a pyromellitic acid or a functional derivative thereof, and (b) an aromatic diamine component consisting essentially of, based on the total amount of the aromatic diamine component, 30 to 100 mole % of a phenylenediamine and 0 to 70 mole % of a diaminodiphenyl ether.
Claim 3
Dependent Claim
57 words
An aromatic polyamic acid solution composition according to claim 1 wherein the aromatic tetracarboxylic acid component comprises, based on the total amount of the aromatic tetracarboxylic acid component, 20 to 85 mole % of a biphenyltetracarboxylic acid or a functional derivtive thereof and 15 to 80 mole % of a pyromellitic acid or a functional derivative thereof.
Claim 4
Dependent Claim
57 words
An aromatic polyamic acid solution composition according to claim 1 wherein the aromatic tetracarboxylic acid component comprises, based on the total amount of the aromatic tetracarboxylic acid component, 25 to 85 mole % of a biphenyltetracarboxylic acid or a functional derivative thereof and 15 to 75 mole % of a pyromellitic acid or a functional derivative thereof.
Claim 5
Dependent Claim
44 words
An aromatic polyamic acid solution composition according to claim 1 wherein the aromatic diamine component comprises, based on the total amount of the aromatic diamine component, 40 to 95 mole % of a phenylenediamine and 5 to 60 mole % of a diaminodiphenyl ether.
Claim 6
Dependent Claim
44 words
An aromatic polyamic acid solution composition according to claim 1 wherein the aromatic diamine component comprises, based on the total amount of the aromatic diamine component, 55 to 90 mole % of a phenylenediamine and 10 to 45 mole % of a diaminodiphenyl ether.
Claim 7
Dependent Claim
40 words
An aromatic polyamic acid solution composition according to claim 1 wherein the biphenyltetracarboxylic acid or functional derivative thereof is selected from the group consisting of 2,3,3',4'-biphenyltetracarboxylic acid and its dianhydride, 3,3',4,4'-biphenyltetracarboxylic acid and its dianhydride, and lower alcohol esters thereof.
Claim 8
Dependent Claim
34 words
An aromatic polyamic acid solution composition according to claim 1 wherein the pyromellitic acid or functional derivative thereof is selected from the group consisting of pyromellitic acid, its dianhydride and its lower alcohol ester.
Claim 9
Dependent Claim
23 words
An aromatic polyamic acid solution composition according to claim 1 wherein the phenylenediamine is selected from the group consisting of 1,4-diaminobenzene-(p-phenylenediamine),1,3-diaminobenzene and 1,2-diaminobenzene.
Claim 10
Dependent Claim
28 words
An aromatic polyamic acid solution composition according to claim 1 wherein the diaminodiphenyl ether is selected from the group consisting of 4,4'-diaminodiphenyl ether, 3,3'-diaminodiphenyl ether and 3,4'-diaminodiphenyl ether.
Claim 11
Dependent Claim
45 words
An aromatic polyamic acid solution composition according to claim 1 wherein the aromatic polyamic acid has a logarithmic viscosity number of about 0.1 to about 5 as determined at 30° C. with respect to an N-methyl-2-pyrrolidone solution having a polymer concentration of 0.5 g/100 ml.
Claim 12
Dependent Claim
40 words
An aromatic polyamic acid solution composition according to claim 1 wherein the polymerization of the aromatic tetracarboxylic acid component and the aromatic diamine component is carried out at a temperature not higher than 100° C. in an organic polar solvent.
Claim 13
Dependent Claim
32 words
An aromatic polyamic acid solution composition according to claim 1 wherein the organic polar solvent is selected from the group consisting of N-methyl-2-pyrrolidone, dimethylsulfoxide, N,N-dimethylacetamide, N,N-dimethylformamide, N,N-diethylacetamide, N,N-diethylformamide, dimethylsulfone and mixtures thereof.
Claim 14
Dependent Claim
31 words
An aromatic polyamic acid solution compositoin according to claim 1 wherein the aromatic polyamic acid is dissolved in an amount of 5 to 35% by weight in the organic polar solvent.
Claim 15
Dependent Claim
27 words
An aromatic oolyamic acid solution composition according to claim 1 which has a rotation viscosity of about 0.1 to about 50000 poise as determined at 30° C.
Claim 16
Dependent Claim
153 words
An aromatic polyimide film. formed by casting or coating in the form of a film an aromatic polyamic acid solution composition comprising an aromatic polyamic acid dissolved in an amount of 5 to 40% by weight in an organic polar solvent, said aromatic polyamic acid being prepared by polymerizing substantially equimolar amounts of an aromatic tetracarboxylic acid component comprising, based on the total amount of the aromatic tetracarboxylic acid component, 15 to 85 mole % of a biphenyltetracarboxylic acid or a functional derivative thereof and 15 to 85 mole % of a pyromellitic acid or a functional derivative thereof and an aromatic diamine component comprising, based on the total amount of the aromatic diamine component, 30 to 100 mole % of a phenylenediamine and 0 to 70 mole % of a diaminodiphenyl ether, and then maintaining the film at a high temperature to remove the organic polar solvent and imidize the polyamic acid.
Claim 17
Dependent Claim
153 words
An aromatic polyimide film. formed by casting or coating in the form of a film an aromatic polyamic acid solution composition comprising an aromatic polyamic acid dissolved in an amount of 5 to 40% by weight in an organic polar solvent, said aromatic polyamic acid being prepared by polymerizing substantially equimolar amounts of an aromatic tetracarboxylic acid component comprising, based on the total amount of the aromatic tetracarboxylic acid component, 15 to 85 mole % of a biphenyltetracarboxylic acid or a functional derivative thereof and 15 to 85 mole % of a pyromellitic acid or a functional derivative thereof and an aromatic diamine component comprising, based on the total amount of the aromatic diamine component, 30 to 100 mole % of a phenylenediamine and 0 to 70 mole % of a diaminodiphenyl ether, and then maintaining the film at a high temperature to remove the organic polar solvent and imidize the polyamic acid.
Claim 18
Dependent Claim
38 words
An aromatic polyimide film according to claim 15 wherein the biphenyltetracarboxylic acid or functional derivative thereof is selected from the group consisting of 2,3,3',4'- biphenyltetracarboxylic acid-and its dianhydride, 3,3',4,4'-biphenyltetracarboxylic acid and its dianhydride, and lower alcohol esters thereof.
Claim 19
Dependent Claim
32 words
An aromatic polyimide film according to claim 15 wherein the pyromellitic acid or functional derivative thereof is selected from the group consisting of pyromellitic acid, its dianhydride and its lower alcohol ester.
Claim 20
Dependent Claim
22 words
An aromatic polyimide film according to claim 15 wherein the phenylenediamine is selected from the group consisting of 1,4-diaminobenzene-(p-phenylenediamine), 1,3-diaminobenzene and 1,2-diaminobenzene.
Claim 21
Dependent Claim
26 words
An aromatic polyimide film according to claim 15 wherein the diaminodiphenyl ether is selected from the group consisting of 4,4'-diaminodiphenyl ether, 3,3'-diaminodiphenyl ether and 3,4'-diminodiphenyl ether.
Claim 22
Dependent Claim
43 words
An aromatic polyimide film according to claim 15 wherein the aromatic polyamic acid has a logarithmic viscosity number of about 1 to about 5 as determined at 30° C. with respect to an N-methyl-2-pyrrolidone solution having a polymer concentration of 0.5 g/100 ml.
Claim 23
Dependent Claim
29 words
An aromatic polyimide film according to claim 15 wherein the organic solvent is selected from the group consisting of N-methyl-2-pyrrolidone, dimethylsulfoxide, N,N-dimethylacetamide, N,N-dimethylformamide, N,N-diethylacetamide, N,N-diethylformamide, dimethylsulfone and mixtures thereof.
Claim 24
Dependent Claim
72 words
An aromatic polyimide film according to claim 15 wherein the cast or coated film having a thickness of about 10 to about 2000 μm is heated gradually at temperatures ranging from about 50° to about 500° C. to solidify the film by evaporating the solvent from the film and then heated to a temperature sufficiently high to imidize the polyamic acid into a polyimide at an imidation degree of at least 90%.
Claim 25
Dependent Claim
48 words
An aromatic polyimide film according to claim 15 which has a second-order transition temperature of at least 300° C., a thermal expansion coefficient of 1.0×10 -5 to 3.0×10 -5 cm/cm/° C., a modulus of elasticity of 300 to 900 kg/mm 2 and an elongation of at least 20%.
Claim 26
Dependent Claim
48 words
An aromatic polyimide film according to claim 15 which has a second-order transition temperature of 305° to 600° C., a thermal expansion coefficient of 1.2×10 -5 to 2.8×10 -5 cm/cm/° C., a modulus of elasticity of 350 to 700 kg/mm 2 and an elongation of 40 to 120%.
Claim 27
Dependent Claim
53 words
A composite sheet comprising a polyimide layer and a metal layer, said polyimide layer having a second-order transition temperature of at least 300° C., a thermal expansion coefficient of 1.0×10 -5 to 3.0×10 -5 cm/cm/° C., a modulus of elasticity of 300 to 900 kg/mm 2 and an elongation of at least 20%.
Claim 28
Dependent Claim
53 words
A composite sheet comprising a polyimide layer and a metal layer, said polyimide layer having a second-order transition temperature of at least 300° C., a thermal expansion coefficient of 1.0×10 -5 to 3.0×10 -5 cm/cm/° C., a modulus of elasticity of 300 to 900 kg/mm 2 and an elongation of at least 20%.
Claim 29
Dependent Claim
105 words
A composite sheet according to claim 25 wherein said polyimide layer is formed from an aromatic polyamic acid prepared by polymerizing substantially equimolar amounts of an aromatic tetracarboxylic acid component comprising, based on the total amount of the aromatic tetracarboxylic acid component, 15 to 85 mole % of a biphenyltetracarboxylic acid or a functional derivative thereof and 15 to 85 mole % of a pyromellitic acid or a functional derivative thereof, and an aromatic diamine component comprising, based on the total amount of the aromatic diamine component, 30 to 100 mole % of a phenylenediamine and 0 to 70 mole % of a diaminodiphenyl ether.
Claim 30
Dependent Claim
50 words
A composite sheet according to claim 25 wherein said polyimide layer has a second-order transition temperature of 305° to 600° C., a thermal expansion coefficient of 1.2×10 -5 to 2.8×10 -5 cm/cm/° C., a modulus of elasticity of 350 to 700 kg/mm 2 and an elongation of 40 to 120%.
References Cited (Backward Citations)
USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
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| 3.5 Years (Year 4) | 1991-10-18 | 1992-04-18 | 1992-10-18 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1995-10-18 | 1996-04-18 | 1996-10-18 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1999-10-18 | 2000-04-18 | 2000-10-18 | $7700.00 | Window Closed / Lapsed |