US4460638A
Expired / Lapsed
US
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Fiber reinforced glass matrix composites
Assignee: Dow Silicones Corp
•
Filing: 1983-04-06
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Granted: 1984-07-17
•
Expires: 2003-04-06
Abstract
Abstract What is disclosed is a method of preparing fiber reinforced glass composites from high modulus fibers, such as carbon fibers and silicon carbide fibers, and silazane polymers. The composites are obtained by heating a pressed and post-cured prepreg to an elevated temperature in an inert atmosphere. Prepregs containing silicon carbide fibers can be fired in air. A simple, low temperature laminating procedure is used in the preparation of these composites in place of the standard hot pressing technique.
Inventors
- 👤 Loren A. Haluska
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-10-25 06:00
CPC Classifications
C; C03; C03C; C03C14/00; C03C14/002; C03C2214/00; C03C2214/02; Y; Y10; Y10S; Y10S428/00; Y10S428/902; Y10T; Y10T428/00; Y10T428/29; Y10T428/2913; Y10T428/2918; Y10T428/2933; Y10T428/2962; Y10T428/30; Y10T428/31504; Y10T428/31652; Y10T428/31663; Y10T442/00; Y10T442/20; Y10T442/2926; Y10T442/2984
Claims Analysis
Total Claims: 66
Claim 1
Independent Claim
122 words
A method of preparing fiber reinforced glass composites which method comprises, (A) impregnating high modulus fibers with a thermosetting silazane polymer dissolved in an organic solvent; (B) forming a prepreg by drying the product from (A); (C) pressing the dried product of (B) at an temperature not greater than about 300° C.; (D) curing the pressed prepreg from (C) at a temperature not greater than about 300° C. for a time sufficient to insure complete or nearly complete cross-linking in the prepreg; (E) slowly firing the pressed and cured prepreg from (D) to a temperature of at least 1000° C. in an inert atmosphere or vacuum until a fiber reinforced glass composite is obtained; and (F) cooling the fiber reinforced glass composite.
Claim 2
Independent Claim
122 words
A method of preparing fiber reinforced glass composites which method comprises, (A) impregnating high modulus fibers with a thermosetting silazane polymer dissolved in an organic solvent; (B) forming a prepreg by drying the product from (A); (C) pressing the dried product of (B) at an temperature not greater than about 300° C.; (D) curing the pressed prepreg from (C) at a temperature not greater than about 300° C. for a time sufficient to insure complete or nearly complete cross-linking in the prepreg; (E) slowly firing the pressed and cured prepreg from (D) to a temperature of at least 1000° C. in an inert atmosphere or vacuum until a fiber reinforced glass composite is obtained; and (F) cooling the fiber reinforced glass composite.
Claim 3
Dependent Claim
117 words
A method as described in claim 1 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere, a chlorine-containing disilane or a mixture of chlorine-containing disilanes, of the general formula (Cl.sub.a R.sub.b Si).sub.2 with a disilazane having the general formula (R.sub.3 'Si).sub.2 NH at a temperature in the range of 25° C. to 300° C. while distilling by-produced volatile products, wherein R is vinyl, an alkyl group of 1-3 carbon atoms or the phenyl group; R' is vinyl, hydrogen, an alkyl group of 1-3 carbon atoms or the phenyl group; a has a value of 0.5-3; b has a value of 0-2.5 and the sum of a+b is equal to three.
Claim 4
Dependent Claim
98 words
A method as described in claim 1 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere, an organochlorosilane or a mixture of organochlorosilanes of the general formula R.sub.n SiCl.sub.4-n with a disilazane having the general formula (R.sub.3 'Si).sub.2 NH at a temperature in the range of 25° C. to 300° C. while distilling by-produced volatile products, wherein R is vinyl, an alkyl group of 1-3 carbon atoms or phenyl; R' is vinyl, hydrogen, an alkyl group of 1-3 carbon atoms or phenyl; and n has a value of 1 or 2.
Claim 5
Dependent Claim
141 words
A method as described in claim 1 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere, at a temperature in the range of 25° C. to 370° C. (A) ammonia and (B) chlorine-containing disilanes selected from the group consisting of (i) a chlorine-containing disilane having the general formula [Cl.sub.c R.sub.d Si].sub.2 and (ii) a mixture of chlorine-containing disilanes having the general formula [Cl.sub.e R.sub.f Si].sub.2 wherein c has a value of 1.5-2.0; d has a value of 1.0-1.5; the sum of c+d is equal to three; the ratio of e to f is in the range of 1.1 to 2.1; the sum of e+f is equal to three; and R in each case is selected from a group consisting of the vinyl group, and alkyl radical of 1-3 carbon atoms and the phenyl group.
Claim 6
Dependent Claim
132 words
A method as described in claim 2 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere, a chlorine-containing disilane or a mixture of chlorine-containing disilanes, wherein the number of diorgano-substituted silicon atoms does not exceed the number of monoorgano-substituted silicon atoms, of the general formula (Cl.sub.a R.sub.b Si).sub.2 with a disilazane having the general formula (R.sub.3 'Si).sub.2 NH at a temperature in the range of 125° C. to 300° C. while distilling by-produced volatile products, wherein R is vinyl, an alkyl group of 1-3 carbon atoms or phenyl group; R' is vinyl, hydrogen, an alkyl group of 1-3 carbon atoms or the phenyl group; a has a value of 0.5-3; b has a value of 0-2.5 and the sum of a+b is equal to three.
Claim 7
Dependent Claim
117 words
A method as described in claim 3 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere, an organochlorosilane or a mixture of organochlorosilanes, wherein for said mixture the number of diorgano-substituted silicon atoms does not exceed the number of monoorgano-substituted silicon atoms, of the general formula R.sub.n SiCl.sub.4-n with a disilazane having the general formula (R.sub.3 'Si).sub.2 NH at a temperature in the range of 125° C. to 300° C. while distilling by-produced volatile products, wherein R is vinyl, an alkyl group of 1-3 carbon atoms or phenyl; R' is vinyl, hydrogen, an alkyl group of 1-3 carbon atoms or phenyl; and n has a value of 1 or 2.
Claim 8
Dependent Claim
164 words
A method as described in claim 4 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere at a temperature in the range of 25° C. to 370° C. (A) ammonia and (B) chlorine-containing disilanes selected from the group consisting of (i) a chlorine-containing disilane having the general formula [Cl.sub.c R.sub.d Si].sub.2 and (ii) a mixture of chlorine-containing disilanes having the general formula [Cl.sub.e R.sub.f Si].sub.2 wherein c has a value of 1.5-2.0; d has a value of 1.0-1.5; the sum of c+d is equal to three; the ratio of e to f is in the range of 1.1 to 2.1; the sum of e+f is equal to three; and R in each case is selected from a group consisting of the vinyl group, and alkyl radical of 1-3 carbon atoms and the phenyl group; and wherein the number of diorgano-substituted silicon atoms in the mixture of chlorine-containing disilanes does not exceed the number of monoorgano-substituted silicon atoms.
Claim 9
Dependent Claim
36 words
A method as described in claim 1 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers are essentially undirectional and continuous.
Claim 10
Dependent Claim
36 words
A method as described in claim 2 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers are essentially undirectional and continuous.
Claim 11
Dependent Claim
36 words
A method as described in claim 3 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers are essentially undirectional and continuous.
Claim 12
Dependent Claim
36 words
A method as described in claim 4 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers are essentially undirectional and continuous.
Claim 13
Dependent Claim
36 words
A method as described in claim 5 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers are essentially undirectional and continuous.
Claim 14
Dependent Claim
36 words
A method as described in claim 6 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers are essentially undirectional and continuous.
Claim 15
Dependent Claim
36 words
A method as described in claim 7 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers are essentially undirectional and continuous.
Claim 16
Dependent Claim
35 words
A method as described in claim 1 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers form a woven fabric.
Claim 17
Dependent Claim
35 words
A method as described in claim 2 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers form a woven fabric.
Claim 18
Dependent Claim
35 words
A method as described in claim 3 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers form a woven fabric.
Claim 19
Dependent Claim
35 words
A method as described in claim 4 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers form a woven fabric.
Claim 20
Dependent Claim
35 words
A method as described in claim 5 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers form a woven fabric.
Claim 21
Dependent Claim
35 words
A method as described in claim 6 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers form a woven fabric.
Claim 22
Dependent Claim
35 words
A method as described in claim 7 wherein said high modulus fibers are selected from the group consisting of carbon fibers and silicon carbide fibers and wherein said high modulus fibers form a woven fabric.
Claim 23
Dependent Claim
25 words
A method as described in claim 1 wherein the prepreg of step (B) pressed in step (C) at a temperature of 100° to 300° C.
Claim 24
Dependent Claim
25 words
A method as described in claim 5 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 25
Dependent Claim
25 words
A method as described in claim 6 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 26
Dependent Claim
25 words
A method as described in claim 7 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 27
Dependent Claim
25 words
A method as described in claim 12 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 28
Dependent Claim
25 words
A method as described in claim 13 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 29
Dependent Claim
25 words
A method as described in claim 14 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 30
Dependent Claim
25 words
A method as described in claim 19 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 31
Dependent Claim
25 words
A method as described in claim 20 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 32
Dependent Claim
25 words
A method as described in claim 21 wherein the prepreg of step (D) pressed in step (C) at a temperature of 100° to 300° C.
Claim 33
Dependent Claim
46 words
A process as described in claim 5 wherein said mixture of chlorine-containing disilanes is from the residue of the direct process and wherein in the general formula (Cl a R b Si) 2 and (R 3 'Si) 2 NH, both R and R' are methyl radicals.
Claim 34
Dependent Claim
46 words
A process as described in claim 12 wherein said mixture of chlorine-containing disilanes is from the residue of the direct process and wherein in the general formula (Cl a R b Si) 2 and (R 3 'Si) 2 NH, both R and R' are methyl radicals.
Claim 35
Dependent Claim
46 words
A process as described in claim 19 wherein said mixture of chlorine-containing disilanes is from the residue of the direct process and wherein in the general formula (Cl a R b Si) 2 and (R 3 'Si) 2 NH, both R and R' are methyl radicals.
Claim 36
Dependent Claim
46 words
A process as described in claim 23 wherein said mixture of chlorine-containing disilanes is from the residue of the direct process and wherein in the general formula (Cl a R b Si) 2 and (R 3 'Si) 2 NH, both R and R' are methyl radicals.
Claim 37
Dependent Claim
46 words
A process as described in claim 26 wherein said mixture of chlorine-containing disilanes is from the residue of the direct process and wherein in the general formula (Cl a R b Si) 2 and (R 3 'Si) 2 NH, both R and R' are methyl radicals.
Claim 38
Dependent Claim
46 words
A process as described in claim 29 wherein said mixture of chlorine-containing disilanes is from the residue of the direct process and wherein in the general formula (Cl a R b Si) 2 and (R 3 'Si) 2 NH, both R and R' are methyl radicals.
Claim 39
Dependent Claim
30 words
A method as described in claim 5 wherein the fiber reinforced glass composite of step (G) is subject to steps (A), (B), (D), (E), and (F) one or more times.
Claim 40
Dependent Claim
30 words
A method as described in claim 6 wherein the fiber reinforced glass composite of step (G) is subject to steps (A), (B), (D), (E), and (F) one or more times.
Claim 41
Dependent Claim
30 words
A method as described in claim 7 wherein the fiber reinforced glass composite of step (G) is subject to steps (A), (B), (D), (E), and (F) one or more times.
Claim 42
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 5.
Claim 43
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 6.
Claim 44
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 7.
Claim 45
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 12.
Claim 46
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 13.
Claim 47
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 14.
Claim 48
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 19.
Claim 49
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 20.
Claim 50
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 21.
Claim 51
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 29.
Claim 52
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 30.
Claim 53
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 31.
Claim 54
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 32.
Claim 55
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 37.
Claim 56
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 38.
Claim 57
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 39.
Claim 58
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 40.
Claim 59
Independent Claim
116 words
A method of preparing fiber reinforced glass composites, which method comprises, (A) impregnating silicon carbide fibers with a thermosetting silazane polymer dissolved in an organic solvent; (B) forming a prepreg by drying the product of (A); (C) pressing the dried product of (B) at a temperature of 100° to 300° C.; (D) curing the pressed prepreg from (C) at a temperature not greater than 300° C. for a time sufficient to insure complete or nearly complete cross-linking in the prepreg; (E) slowly firing the pressed and cured prepreg from (D) to a temperature of at least 1000° C. in air until a fiber reinforced glass composite is obtained; and (F) cooling the fiber reinforced glass composite.
Claim 60
Independent Claim
116 words
A method of preparing fiber reinforced glass composites, which method comprises, (A) impregnating silicon carbide fibers with a thermosetting silazane polymer dissolved in an organic solvent; (B) forming a prepreg by drying the product of (A); (C) pressing the dried product of (B) at a temperature of 100° to 300° C.; (D) curing the pressed prepreg from (C) at a temperature not greater than 300° C. for a time sufficient to insure complete or nearly complete cross-linking in the prepreg; (E) slowly firing the pressed and cured prepreg from (D) to a temperature of at least 1000° C. in air until a fiber reinforced glass composite is obtained; and (F) cooling the fiber reinforced glass composite.
Claim 61
Dependent Claim
133 words
A method as described in claim 58 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere, a chlorine-containing disilane or a mixture of chlorine-containing disilanes, wherein the number of diorgano-substituted silicon atoms does not exceed the number of monoorgano-substituted silicon atoms, of the general formula (Cl.sub.a R.sub.b Si).sub.2 with a disilazane having the general formula (R.sub.3 'Si).sub.2 NH at a temperature in the range of 125° C. to 300° C. while distilling by-produced volatile products, wherein R is vinyl, an alkyl group of 1-3 carbon atoms or the phenyl group; R' is vinyl, hydrogen, an alkyl group of 1-3 carbon atoms or the phenyl group; a has a value of 0.5-3; b has a value of 0-2.5 and the sum of a+b is equal to three.
Claim 62
Dependent Claim
117 words
A method as described in claim 58 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere, an organochlorosilane or a mixture of organochlorosilanes, wherein for said mixture the number of diorgano-substituted silicon atoms does not exceed the number of monoorgano-substituted silicon atoms, of the general formula R.sub.n SiCl.sub.4-n with a disilazane having the general formula (R.sub.3 'Si).sub.2 NH at a temperature in the range of 125° C. to 300° C. while distilling by-produced volatile products, wherein R is vinyl, an alkyl group of 1-3 carbon atoms or phenyl; R' is vinyl, hydrogen, an alkyl group of 1-3 carbon atoms or phenyl; and n has a value of 1 or 2.
Claim 63
Dependent Claim
164 words
A method as described in claim 58 wherein said silazane polymer is prepared by contacting and reacting in an inert, essentially anhydrous, atmosphere at a temperature in the range of 25° C. to 370° C. (A) ammonia and (B) chlorine-containing disilanes selected from the group consisting of (i) a chlorine-containing disilane having the general formula [Cl.sub.c R.sub.d Si].sub.2 and (ii) a mixture of chlorine-containing disilanes having the general formula [Cl.sub.e R.sub.f Si].sub.2 wherein c has a value of 1.5-2.0; d has a value of 1.0-1.5; the sum of c+d is equal to three; the ratio of e to f is in the range of 1.1 to 2.1; the sum of e+f is equal to three; and R in each case is selected from a group consisting of the vinyl group, and alkyl radical of 1-3 carbon atoms and the phenyl group; and wherein the number of diorgano-substituted silicon atoms in the mixture of chlorine-containg disilanes does not exceed the number of monoorgano-substituted silicon atoms.
Claim 64
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 59.
Claim 65
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 60.
Claim 66
Dependent Claim
13 words
A fiber reinforced glass composite as prepared by the method of claim 61.
References Cited (Backward Citations)
No citation records indexed.
USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 1987-07-17 | 1988-01-16 | 1988-07-17 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1991-07-17 | 1992-01-16 | 1992-07-17 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1995-07-17 | 1996-01-16 | 1996-07-17 | $7700.00 | Window Closed / Lapsed |