EP0045499A2
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EP
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Novel wholly aromatic copolyester, process for production thereof, and film melt-shaped therefrom
Assignee: Teijin Ltd
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Filing: 1981-07-31
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Granted: —
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Expires: 2001-07-31
Abstract
Abstract A wholly aromatic copolyester composed mainly of isophthalic acid units and hydroquinone units, the total proportion of said isophthalic acid units and hydroquinone units being at least about 80 mole% based on the entire units, said wholly aromatic copolyester having a terminal carboxyl group concentration, measured by the method described in the specification, of not more than about 90 eq/10 6 g and a reduced viscosity, determined at 35°C in a mixed solvent of phenol and tetrachloroethane in a weight ratio of 4:6 in a concentration of 1.2 gfdl of at least about 0.6 and being substantially linear and melt-shapable and substantially free from a halogen atom bonded to the molecular chain, and a film prepared therefrom by melt shaping. The wholly aromatic copolyester can be prepared by a process which comprises polycondensing under heat in the presence of a polycondensation catalyst (a) a reaction mixture consisting of a major proportion of a diaryl ester of isophthalic acid and hydroquinone and a minor proportion of at least one other component selected from diaryl esters of aromatic dicarboxylic acids other than isophthalic acid, aromatic dihydroxy compounds other than hydroquinone and aryl hydroxyenboates or (b) a reaction mixture consisting of a major proportion of isophthalic acid, hydroquinone and a diaryl carbonate and a minor proportion of at least one other component selected from aromatic dicarboxylic acids other than isophthalic acid, aromatic dihydroxy compounds other than hydroquinone, hydroxybenzoic acid and aryl hydroxybenzoates, and after the reduced viscosity of the polymer formed in the reaction system has reached about 0.2, performing the polycondensation at a temperature lower than the crystalline melting point of the polymer while maintaining the reaction system in a molten condition; or which comprises polymerizing the wholly aromatic copolyester having a reduced viscosity of at least 0.6 prepared by the above process or a wholly aromatic copolyester having a reduced viscosity of less than about 0.6 in the solid phase in a manner known per se under reduced pressure or while passing an inert gas into the reaction system. The film can be used as films for metal vapor depocition, films for printed circuits and electrical insulating films by using their excellent heat resistance.
Inventors
- 👤 Takanori Urasaki
- 👤 Tugusi Yoshida
- 👤 Hiroo Inata
- 👤 Yasuji Hirabayashi
Bibliographic Details
Application Number
—
Jurisdiction
EP
Data Source
google_patents
Last Synchronized
2026-11-03 07:41
CPC Classifications
C; C08; C08J; C08J5/00; C08J5/18; C08G; C08G63/00; C08G63/02; C08G63/12; C08G63/16; C08G63/18; C08G63/19; C08G63/60; C08G63/605; C08G63/64; C08G63/66; C08G63/668; C08G63/672; C08J2367/00; C08J2367/02; C08J2367/03
Claims Analysis
Total Claims: 34
Claim 1
Independent Claim
113 words
A wholly aromatic copolyester composed mainly of isophthalic acid units and hydroquinone units, the total proportion of said isophthalic acid units and hydroquinone units being at least about 80 mole% based on.the entire units, said wholly aromatic copolyester having a terminal carboxyl group concentration, measured by the method described in the specification, of not more than about 90 eq/ 1 0 6 g and a reduced viscosity, determined at 35°C in a mixed solvent of phenol and tetrachloroethane in a weight ratio of 4:6 in a concentration of 1.2 g/dl of at least about 0.6 and being substantially linear and melt-shapable and substantially free from a halogen atom bonded to the molecular chain.
Claim 2
Dependent Claim
113 words
A wholly aromatic copolyester composed mainly of isophthalic acid units and hydroquinone units, the total proportion of said isophthalic acid units and hydroquinone units being at least about 80 mole% based on.the entire units, said wholly aromatic copolyester having a terminal carboxyl group concentration, measured by the method described in the specification, of not more than about 90 eq/ 1 0 6 g and a reduced viscosity, determined at 35°C in a mixed solvent of phenol and tetrachloroethane in a weight ratio of 4:6 in a concentration of 1.2 g/dl of at least about 0.6 and being substantially linear and melt-shapable and substantially free from a halogen atom bonded to the molecular chain.
Claim 3
Dependent Claim
30 words
The wholly aromatic copolyester of claim 1 wherein the total proportion of the isophthalic acid units and hydroquinone units is about 85 to about 95 mole% of the entire units.
Claim 4
Dependent Claim
186 words
The wholly aromatic copolyester of claim 1 or 2 which is composed substantially of the isophthalic acid units and hydroquinone units and at least one type of units selected from the group consisting of bisphenol units of the following formula wherein X is -0-, >C=O or in which R 1 and R 2 are identical or different and each represents a hydrogen atom, a methyl group, an ethyl group or a phenyl group, or R 1 and R 2 taken, together with the carbon atom to which they are bonded, may form a cyclohexane ring, substituted hydroquinone units of the following formula wherein R 3 represents a tertiary alkyl group having 4 to 9 carbon atoms or a phenyl group which may be substituted by a tertiary butyl group, substituted or unsubstituted resorcinol units of the following formula wherein R represents a hydrogen atom, a tertiary alkyl group having 4 to 9 carbon atoms, or a phenyl group which may be substituted by a tertiary butyl group, and hydroxybenzoic acid units of the following formula wherein -0- and -CO- are meta or para to each other.
Claim 5
Dependent Claim
31 words
The wholly aromatic copolyester of claim 3 which consists substantially of isophthalic acid units, hydroquinone units, and the bisphenol units of formula (1) and/or the substituted hydroquinone units of formula (2).
Claim 6
Dependent Claim
28 words
The wholly aromatic copolyester of any one of claims 1 to 4 which has a terminal carboxyl group concentration of about 5 to about 70 eq/10 6 g.
Claim 7
Dependent Claim
23 words
The wholly aromatic copolyester of any one of claims 1 to 5 which has a reduced viscosity of about 0.7 to about 210.
Claim 8
Dependent Claim
41 words
7, The wholly aromatic copolyester of claim 1 wherein a halogen atom bonded to the molecular chain is a halogen atom at the terminal of the molecular chain, or a halogen atom bonded to the aromatic ring in the molecular chain.
Claim 9
Dependent Claim
31 words
The wholly aromatic copolyester of claim 1 which has a flow index, at a shear rate of about 50 to about 500 sec -1 of 0.7 to 0.9 on an average.
Claim 10
Dependent Claim
136 words
A process for producing the wholly aromatic copolyester defined in claim 1 or a wholly aromatic copolyester having a reduced viscosity of less than about 0.6, which comprises polycondensing under heat in the presence of a polycondensation catalyst a reaction mixture consisting of a major proportion of a diaryl ester of isophthalic acid and hydroquinone and a minor proportion of at least one other component selected from diaryl esters of aromatic dicarboxylic acids other than isophthalic acid, aromatic dihydroxy compounds other than hydroquinone and aryl hydroxyenboates while intermittently or continuously removing the hydroxyaryl compound formed, and after the reduced viscosity of the polymer formed in the reaction system has reached about 0.2, performing the polycondensation at a temperature lower than the crystalline melting point of the polymer while maintaining the reaction system in a molten condition.
Claim 11
Dependent Claim
137 words
A process for producing the wholly aromatic copolyester defined in claim 1 or a wholly aromatic copolyester having a reduced viscosity of less than about 0.6, which comprises polycondensing under heat in the presence of a polycondensation catalyst a reaction mixture consisting of a major proportion of isophthalic acid, hydroquinone and a diaryl carbonate and a minor proportion of at least one other component selected from aromatic dicarboxylic acids other than isophthalic acid, aromatic dihydroxy compounds other than hydroquinone, hydroxybenzoic acid and aryl hydroxybenzoates while intermittently or continuously removing the hydroxyaryl compound and carbon dioxide formed, and after the reduced viscosity of the polymer formed in the reaction system has reached about 0.2, performing the polycondensation at a temperature lower than the crystalline melting point of the polymer while maintaining the reaction system in a molten conditions.
Claim 12
Dependent Claim
32 words
ll. The process of claim 9 or 10 wherein when the reduced viscosity of the polymer formed in the reaction system has reached about 0.08, the reaction system is under reduced pressure.
Claim 13
Dependent Claim
42 words
The process of claim 9 or 10 wherein at least until the reduced viscosity of the polymer formed in the reaction system reaches about 0.15, the polycondensation is carried out at a temperature higher than the crystalline melting point of the polymer.
Claim 14
Dependent Claim
66 words
A process for producing the wholly aromatic copolyester defined in claim 1 whose reduced viscosity has been enhanced, which comprises polymerizing the wholly aromatic copolyester defined in claim 1 or w wholly aromatic copolyester having a reduced viscosity of less than about 0.6 in the solid phase in a manner known per se under reduced pressure or while passing an inert gas into the reaction system.
Claim 15
Dependent Claim
115 words
A film prepared by melt shaping from a wholly aromatic copolyester composed mainly of isophthalic acid units and hydroquinone units,said wholly aromatic copolyester comprising at least about 80 mole%, based on the entire units, of the isophthalic acid units and hydroquinone units, said copolyester having a terminal carboxyl group, measured by the method described in the specification, of not more than about 90 eq 10 6 g and a reduced viscosity, determined at 35°C in a mixed solvent of phenol and tetrachloroethane in a weight ratio of 4:6 in a concentration of 1.2 g/dl, of at least about 0.6 and being substantially linear and substantially free from a halogen atom bonded to the molecular chain.
Claim 16
Dependent Claim
115 words
A film prepared by melt shaping from a wholly aromatic copolyester composed mainly of isophthalic acid units and hydroquinone units,said wholly aromatic copolyester comprising at least about 80 mole%, based on the entire units, of the isophthalic acid units and hydroquinone units, said copolyester having a terminal carboxyl group, measured by the method described in the specification, of not more than about 90 eq 10 6 g and a reduced viscosity, determined at 35°C in a mixed solvent of phenol and tetrachloroethane in a weight ratio of 4:6 in a concentration of 1.2 g/dl, of at least about 0.6 and being substantially linear and substantially free from a halogen atom bonded to the molecular chain.
Claim 17
Dependent Claim
8 words
The film of claim 14 which is unstretched.
Claim 18
Dependent Claim
8 words
The film of claim 14 which is stretched.
Claim 19
Dependent Claim
9 words
The film of claim 16 which is biaxially stretched.
Claim 20
Dependent Claim
47 words
The film of any one of claims 14 to 17 which has within its plane two perpendicularly crossing directions each of which has a Young's modulus of at least about 70 kg / mm 2 and a strength of at least about 7 kg/mm 2 at 25°C.
Claim 21
Dependent Claim
99 words
The film of claim 14, 16, or 17, or 18 according to claim 16 or 17 which has a coefficient of linear expansion, defined by the following formula, of not more than about 8 x 10 -5 mm/mm/°C. wherein L 260 is the film length (mm) attained when a film sample having a length of about 100 mm and a width of about 5 mm at 25°C is heated at 260°C under no tension, and L 25 is the film length (mm) attained when the film used in the measurement of L 260 is allowed to cool to 25°C.
Claim 22
Dependent Claim
78 words
The film of any one of claims 14 to 19 which has a heat shrinkage (%), defined by the following formula, of not more than about 5%: wherein ℓ 25 is the length (cm) of the film at 25°C, and ℓ 260 is the film length (cm) attained when the film sample used for the measurement of ℓ 25 is heated at 260 ° C for 60 seconds under no tension and then allowed to cool to 25°C.
Claim 23
Dependent Claim
16 words
The film of claim 20 which has a heat shrinkage of not more than about 1%.
Claim 24
Dependent Claim
21 words
The film of any one of claims 14 to 21 which has an elongation at 25°C of at least about 20%.
Claim 25
Dependent Claim
26 words
The film of claim 22 which has an elongation at 25°C of at least about 20% when heat-treated at 260°C for 60 seconds under no tension.
Claim 26
Dependent Claim
59 words
A process for producing a film from the wholly aromatic copolyester defined in claim 1 by melt shaping, which comprises heating the wholly aromatic copolyester to the melt-shapable temperature, extruding the molten copolyester from a slit, then if desired monoaxially or biaxially stretching the extrudate, then if desired heat-setting the film, and then if desired heat shrinking the film.
Claim 27
Dependent Claim
26 words
The process of claim 24 wherein the melt-shapable temperature is between a point higher than the melting point of the wholly aromatic copolyester and about 400°C.
Claim 28
Dependent Claim
13 words
The process of claim 24 wherein the biaxial stretching is carried out successively.
Claim 29
Dependent Claim
15 words
The process of claim 24 wherein the heat-setting is carried out substantially at constant length.
Claim 30
Dependent Claim
14 words
The process of claim 24 wherein the heat shrinking is carried out under tension.
Claim 31
Dependent Claim
97 words
The process of claim 24 which comprises heating the wholly aromatic polyester defined in claim 1 to a temperature above the melt-shapable temperature, extruding the molten polyester through a slit, then biaxially stretching the unstretched film at about 180 to about 280°C either successively or simultaneously, heat-setting the biaxially stretched film substantially at constant length at a temperature between a temperature about 20°C lower than the melting point of the copolyester and about 250°C, and then if desired, shrinking the film under tension at a temperature lower than the temperature used in the heat-setting and about 200°C.
Claim 32
Dependent Claim
21 words
The process of claim 29 wherein the biaxial stretching is carried out at a temperature of about 185 to about 250°C.
Claim 33
Dependent Claim
33 words
The process of claim 29 or 30 wherein the biaxial stretching is carried out so that the refractive index of the film is at least about 1.62 in both of the stretching directions.
Claim 34
Dependent Claim
28 words
The process of any one of claims 29 to 31 wherein the biaxial stretching is carried out so that the area ratio is about 2.8 to about 10.
References Cited (Backward Citations)
No citation records indexed.
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