US4110302A
Expired / Lapsed
US
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Reinforced polycarbodiimide modified polyalkylene terephthalate
Assignee: Celanese Corp
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Filing: 1977-03-07
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Granted: 1978-08-29
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Expires: 1997-03-07
Abstract
Abstract Molding resin compositions comprising a polycarbodiimide modified polyalkylene terephthalate polymer (polypropylene terephthalate, polybutylene terephthalate, or mixtures thereof) and a reinforcing agent such as glass fibers have been found to exhibit improved impact strength and thus are useful in various molding applications in order to prepare articles of manufacture having, e.g., industrial (e.g., gears, bearings), automotive (e.g., automotive distributor caps, distributor rotors), and electrical (e.g., motor end caps, brush holders) applications. These molding resin compositions are particularly useful in certain automotive, industrial, and electrical applications where greater impact strength may be required to extend the useful life of various articles of manufacture which may be subjected to occasional or continuous shock or impact. These molding resin compositions may be prepared by intimately admixing in the molten state a reinforcing agent such as glass fibers with a polycarbodiimide modified polyalkylene terephthalate polymer formed from the reaction between a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, and a polycarbodiimide which is both (1) derived from at least one aromatic diisocyanate which is either unsubstituted or contains up to one methyl substituent on each aromatic ring, and (2) contains at least two carbodiimide units per polycarbodiimide molecule. The components of the composition are preferably prepared by charging the polyalkylene terephthalate to the hopper of a melt screw extruder and adding the polycarbodiimide and reinforcing agent downstream in the extruder--e.g., in the vent port or other side feed port of the extruder.
Inventors
- 👤 Norman W. Thomas
- 👤 Frank M. Berardinelli
- 👤 Robert Edelman
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-10-23 22:56
CPC Classifications
C; C08; C08G; C08G69/00; C08G69/44; C08K; C08K3/00; C08K3/34; C08K3/40; C08L; C08L1/00; C08L101/00; C08L67/00; C08L67/02; C08L79/00
Claims Analysis
Total Claims: 24
Claim 1
Independent Claim
148 words
In a process for producing a reinforced polyalkylene terephthalate molding resin composition comprising intimately mixing in the molten state a reinforcing agent with a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.2 to about 1.2 deciliters per gram, the improvement comprising modifying said polyalkylene terephthalate polymer by reacting the polyalkylene terephthalate polymer in the molten state with at least one polycarbodiimide, which polycarbodiimide both (1) is derived from at least one aromatic diisocyanate which is either unsubstituted or contains up to one methyl substituent on each aromatic ring, and (2) contains at least two carbodiimide units per polycarbodiimide molecule, whereby said resulting molding resin composition exhibits a substantially improved impact strength.
Claim 2
Dependent Claim
148 words
In a process for producing a reinforced polyalkylene terephthalate molding resin composition comprising intimately mixing in the molten state a reinforcing agent with a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.2 to about 1.2 deciliters per gram, the improvement comprising modifying said polyalkylene terephthalate polymer by reacting the polyalkylene terephthalate polymer in the molten state with at least one polycarbodiimide, which polycarbodiimide both (1) is derived from at least one aromatic diisocyanate which is either unsubstituted or contains up to one methyl substituent on each aromatic ring, and (2) contains at least two carbodiimide units per polycarbodiimide molecule, whereby said resulting molding resin composition exhibits a substantially improved impact strength.
Claim 3
Dependent Claim
31 words
The process of claim 1 wherein said reaction between the polycarbodiimide and the polyalkylene terephthalate polymer takes place simultaneously with the mixing of the polyalkylene terephthalate polymer and the reinforcing agent.
Claim 4
Dependent Claim
49 words
The process of claim 1 wherein there is employed from about 0.1 to about 5% by weight polycarbodiimide, from about 40 to about 85% by weight polyalkylene terephthalate, and from about 15 to about 60% by weight reinforcing agent based upon the total weight of the reinforced resin composition.
Claim 5
Dependent Claim
27 words
The process of claim 2 wherein said reaction is carried out at a temperature of from about 220° to about 300° C and at substantially atmospheric pressure.
Claim 6
Dependent Claim
31 words
The process of claim 4 wherein said polycarbodiimide may be selected from the group consisting of poly(tolyl carbodiimide), poly(4,4'-diphenylmethane carbodiimide), poly(3,3'-dimethyl-4,4'-biphenylene carbodiimide), poly(p-phenylene carbodiimide), poly(m-phenylene carbodiimide), poly(3,3'-dimethyl-4,4'-diphenylmethane carbodiimide) and mixtures thereof.
Claim 7
Dependent Claim
28 words
The process of claim 5 wherein the reinforcing agents may be selected from the group consisting of glass fibers, asbestos fibers, cellulosic fibers, synthetic fibers, and mixtures thereof.
Claim 8
Dependent Claim
173 words
In a process for producing a reinforced polyalkylene terephthalate molding resin composition comprising intimately mixing in the molten state from about 20 to about 50% by weight of a reinforcing agent with from about 50 to about 80% by weight of a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.5 to about 1.0 deciliters per gram, the improvement comprising modifying said polyalkylene terephthalate polymer by reacting said polymer in the molten state with from about 0.2 to about 4% by weight of at least one polycarbodiimide, which polycarbodiimide both (1) is derived from at least one aromatic diisocyanate which is either unsubstituted or contains up to one methyl substituent on each aromatic ring, and (2) contains at least two carbodiimide units per polycarbodiimide molecule, whereby said resulting molding resin composition exhibits a substantially improved impact strength.
Claim 9
Dependent Claim
173 words
In a process for producing a reinforced polyalkylene terephthalate molding resin composition comprising intimately mixing in the molten state from about 20 to about 50% by weight of a reinforcing agent with from about 50 to about 80% by weight of a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.5 to about 1.0 deciliters per gram, the improvement comprising modifying said polyalkylene terephthalate polymer by reacting said polymer in the molten state with from about 0.2 to about 4% by weight of at least one polycarbodiimide, which polycarbodiimide both (1) is derived from at least one aromatic diisocyanate which is either unsubstituted or contains up to one methyl substituent on each aromatic ring, and (2) contains at least two carbodiimide units per polycarbodiimide molecule, whereby said resulting molding resin composition exhibits a substantially improved impact strength.
Claim 10
Dependent Claim
31 words
The process of claim 7, wherein the reaction between the polycarbodiimide and the polyalkylene terephthalate polymer takes place simultaneously with the mixing of the polyalkylene terephthalate polymer and the reinforcing agent.
Claim 11
Dependent Claim
76 words
The process of claim 7 wherein said polycarbodiimide may be selected from the group consisting of poly(tolyl carbodiimide), poly(4,4'-diphenylmethane carbodiimide), poly(3,3'-dimethyl-4,4-biphenylene carbodiimide), poly(p-phenylene carbodiimide), poly(m-phenylene carbodiimide), poly(3,3'-dimethyl-4,4'-diphenylmethane carbodiimide) and mixtures thereof, said reinforcing agent may be selected from the group consisting of glass fibers, asbestos fibers, cellulosic fibers, synthetic fibers, and mixtures thereof, and wherein said reaction is carried out at a temperature of from about 225° to about 275° C and at substantially atmospheric pressure.
Claim 12
Dependent Claim
172 words
In a process for producing a reinforced polyalkylene terephthalate molding resin composition comprising intimately mixing in the molten state from about 25 to about 40% by weight of a reinforcing agent with from about 60 to about 75% by weight of a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.5 to about 1.0 deciliters per gram, the improvement comprising modifying said polyalkylene terephthalate polymer by reacting said polymer in the molten state with from about 0.3 to about 3% by weight of at least one polycarbodiimide selected from the group consisting of poly(tolyl carbodiimide), poly(4,4'-diphenylmethane carbodiimide), poly(3,3'-dimethyl-4,4'-biphenylene carbodiimide), poly(p-phenylene carbodiimide), poly(m-phenylene carbodiimide), poly(3,3'-dimethyl-4,4'-diphenylmethane carbodiimide), and mixtures thereof at a temperature of from about 230° to about 260° C and at substantially atmospheric pressure whereby said resulting molding resin composition exhibits a substantially improved impact strength.
Claim 13
Dependent Claim
172 words
In a process for producing a reinforced polyalkylene terephthalate molding resin composition comprising intimately mixing in the molten state from about 25 to about 40% by weight of a reinforcing agent with from about 60 to about 75% by weight of a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.5 to about 1.0 deciliters per gram, the improvement comprising modifying said polyalkylene terephthalate polymer by reacting said polymer in the molten state with from about 0.3 to about 3% by weight of at least one polycarbodiimide selected from the group consisting of poly(tolyl carbodiimide), poly(4,4'-diphenylmethane carbodiimide), poly(3,3'-dimethyl-4,4'-biphenylene carbodiimide), poly(p-phenylene carbodiimide), poly(m-phenylene carbodiimide), poly(3,3'-dimethyl-4,4'-diphenylmethane carbodiimide), and mixtures thereof at a temperature of from about 230° to about 260° C and at substantially atmospheric pressure whereby said resulting molding resin composition exhibits a substantially improved impact strength.
Claim 14
Dependent Claim
120 words
A reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition having improved impact strength, said resin comprising a reinforcing agent intimately admixed with the reaction product of (a) a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.2 to about 1.2 deciliters per gram, and (b) a polycarbodiimide which both (1) is derived from at least one aromatic diisocyanate which is either unsubstituted or contains up to one methyl substituent on each aromatic ring, and (2) contains at least two carbodiimide units per polycarbodiimide molecule.
Claim 15
Dependent Claim
120 words
A reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition having improved impact strength, said resin comprising a reinforcing agent intimately admixed with the reaction product of (a) a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.2 to about 1.2 deciliters per gram, and (b) a polycarbodiimide which both (1) is derived from at least one aromatic diisocyanate which is either unsubstituted or contains up to one methyl substituent on each aromatic ring, and (2) contains at least two carbodiimide units per polycarbodiimide molecule.
Claim 16
Dependent Claim
36 words
The reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition of claim 11 wherein there is employed from about 15 to about 60% by weight reinforcing agent based upon the total weight of the reinforced resin composition.
Claim 17
Dependent Claim
19 words
The reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition of claim 12 wherein said reinforcing agent is glass fibers.
Claim 18
Dependent Claim
20 words
The reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition of claim 12 wherein said reinforcing agent is acicular calcium metasilicate.
Claim 19
Dependent Claim
34 words
The reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition of claim 13 wherein said polyalkylene terephthalate polymer is polybutylene terephthalate having an intrinsic viscosity of from about 0.5 to about 1.0 deciliters per gram.
Claim 20
Dependent Claim
37 words
The reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition of claim 11 wherein said polycarbodiimide is selected from the group consisting of poly(tolyl carbodiimide), poly(4,4'-diphenylmethane carbodiimide), poly(3,3'-dimethyl-4,4'-biphenylene carbodiimide), poly(p-phenylene carbodiimide), poly(m-phenylene carbodiimide), poly(3,3'-dimethyl-4,4'-diphenylmethane carbodiimide) and mixtures thereof.
Claim 21
Dependent Claim
62 words
The reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition of claim 16 wherein said reinforced polycarbodiimide modified polyalkylene terephthalate composition comprises from about 0.1 to about 5% by weight polycarbodiimide, from about 40 to about 85% by weight polyalkylene terephthalate polymer, and from about 15 to about 60% by weight reinforcing agent based upon the total weight of the reinforced resin composition.
Claim 22
Dependent Claim
118 words
A reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition comprising from about 20 to about 50% by weight of a reinforcing agent intimately admixed with the reaction product of (a) from about 50 to about 80% by weight of a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.5 to about 1.0 deciliters per gram, and (b) from about 0.2 to about 4% by weight of a polycarbodiimide selected from the group consisting of poly(tolyl carbodiimide), poly (4,4'-diphenylmethane carbodiimide), and mixtures thereof.
Claim 23
Dependent Claim
118 words
A reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition comprising from about 20 to about 50% by weight of a reinforcing agent intimately admixed with the reaction product of (a) from about 50 to about 80% by weight of a polyalkylene terephthalate polymer which is the reaction product of terephthalic acid or a dialkyl ester of terephthalic acid and a glycol selected from the group consisting of trimethylene glycol, tetramethylene glycol, and mixtures thereof, said polyalkylene terephthalate having an intrinsic viscosity of from about 0.5 to about 1.0 deciliters per gram, and (b) from about 0.2 to about 4% by weight of a polycarbodiimide selected from the group consisting of poly(tolyl carbodiimide), poly (4,4'-diphenylmethane carbodiimide), and mixtures thereof.
Claim 24
Dependent Claim
31 words
The reinforced polycarbodiimide modified polyalkylene terephthalate molding resin composition of claim 18 wherein said reinforcing agent is glass, said polyalkylene terephthalate polymer is polybutylene terephthalate, and said polycarbodiimide is poly(4,4'-diphenylmethane carbodiimide).
References Cited (Backward Citations)
USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 1981-08-28 | 1982-02-27 | 1982-08-29 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1985-08-28 | 1986-02-27 | 1986-08-29 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1989-08-28 | 1990-02-27 | 1990-08-29 | $7700.00 | Window Closed / Lapsed |