US4772516A
Expired / Lapsed
US
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Stable methylpolydisilylazane polymers
Assignee: Individual
•
Filing: 1987-11-09
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Granted: 1988-09-20
•
Expires: 2007-11-09
Abstract
Abstract A method for producing methylpolydisilylazane polymers of reduced chloride content that exhibit no increase in pyrophoricity and exhibit improved shelf life. The methylpolydisilylazane polymers of reduced chloride content are useful in the production of silicon nitride and sil STATEMENT OF GOVERNMENT RIGHTS The United States Government has rights in this invention pursuant to Contract Number F33615-85-C-5006 awarded by the United States Air Force.
Inventors
- 👤 Louis G. Mahone
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-06 15:23
CPC Classifications
C; C04; C04B; C04B41/00; C04B41/009; C01; C01B; C01B21/00; C01B21/06; C01B21/068; C01B32/00; C01B32/90; C01B32/914; C01B32/956; C01B32/963; C01B32/977; C04B35/00; C04B35/515; C04B35/56; C04B35/565; C04B35/571; C04B35/58; C04B35/584; C04B35/589; C04B41/45; C04B41/50; C04B41/5053; C04B41/5062; C04B41/5066; C04B41/80; C04B41/81; C04B41/85; C04B41/87; C08; C08G; C08G77/00; C08G77/60; C08G77/62; C01P; C01P2006/00; C01P2006/80; Y; Y10; Y10S; Y10S521/00; Y10S521/919; Y10T; Y10T428/00; Y10T428/30; Y10T428/31504; Y10T428/31652; Y10T428/31663
Claims Analysis
Total Claims: 33
Claim 1
Independent Claim
69 words
A method of preparing a stable methylpolydisilylazane polymer with reduced chloride content and without increased pyrophoricity, which method comprises the steps of: (a) dissolving about 15 weight percent to about 80 weight percent solids of said polymer in an organic solvent; (b) contacting the dissolved polymer with ammonia; (c) reacting the dissolved polymer with said ammonia for about 1 to about 20 hours; and (d) recovering the reacted polymer.
Claim 2
Independent Claim
69 words
A method of preparing a stable methylpolydisilylazane polymer with reduced chloride content and without increased pyrophoricity, which method comprises the steps of: (a) dissolving about 15 weight percent to about 80 weight percent solids of said polymer in an organic solvent; (b) contacting the dissolved polymer with ammonia; (c) reacting the dissolved polymer with said ammonia for about 1 to about 20 hours; and (d) recovering the reacted polymer.
Claim 3
Dependent Claim
15 words
A method as recited in claim 1 wherein said ammonia is in the gaseous phase.
Claim 4
Dependent Claim
15 words
A method as recited in claim 1 wherein said ammonia is in the liquid phase.
Claim 5
Dependent Claim
27 words
A method as recited in claim 2 wherein: said reacting step is conducted at a temperature in the range of about -34° C. to about 70° C.
Claim 6
Dependent Claim
22 words
A method as recited in claim 1 wherein: said reacting step is conducted at a temperature above the boiling point of ammonia.
Claim 7
Dependent Claim
20 words
A method as recited in claim 5 wherein: said reacting step is conducted under pressure up to about 100 PSIG.
Claim 8
Dependent Claim
46 words
A method as recited in claim 1 wherein: the chloride content of said methylpolydisilylazane polymer before said contacting step is substantially greater than 0.5 weight percent; and the chloride content of said methylpolydisilylazane polymer is reduced to less than 0.5 weight percent by said reacting step.
Claim 9
Dependent Claim
20 words
A method as recited in claim 1 wherein: said organic solvent is at least one of diethylether, toluene and heptane.
Claim 10
Dependent Claim
38 words
A method as recited in claim 1 wherein: salt is produced as a by-product of said contacting and reacting steps; and said contacting step comprises introducing sufficient ammonia so that the salt by-product is in a liquid phase.
Claim 11
Dependent Claim
38 words
A method as recited in claim 1 wherein: salt is produced as a by-product of said contacting and reacting steps; and said contacting step comprises introducing sufficient ammonia so that the salt by-product is in a solid phase.
Claim 12
Dependent Claim
108 words
A composition of matter consisting essentially of: a methylpolydisilylazane polymer of reduced chloride content represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; said polymer exhibiting no increase in pyrophoricity, as a result of having its chloride content reduced to less than 0.5 weight percent by ammonolysis, compared to the same polymer with greater chloride content prior to chloride reduction by ammonolysis.
Claim 13
Dependent Claim
108 words
A composition of matter consisting essentially of: a methylpolydisilylazane polymer of reduced chloride content represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; said polymer exhibiting no increase in pyrophoricity, as a result of having its chloride content reduced to less than 0.5 weight percent by ammonolysis, compared to the same polymer with greater chloride content prior to chloride reduction by ammonolysis.
Claim 14
Independent Claim
74 words
A method of preparing ceramic materials consisting essentially of silicon, carbon and nitrogen, said method comprising: pyrolyzing methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent.
Claim 15
Independent Claim
74 words
A method of preparing ceramic materials consisting essentially of silicon, carbon and nitrogen, said method comprising: pyrolyzing methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent.
Claim 16
Dependent Claim
19 words
Ceramic materials consisting essentially of silicon, carbon and nitrogen and prepared by the method as claimed in claim 12.
Claim 17
Independent Claim
94 words
A method of preparing a ceramic article consisting essentially of silicon, carbon and nitrogen, said method comprising: (a) forming an article of the desired shape from a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; wherein the average chloride content of said polymer being less than 0.5 weight percent; and (b) pyrolyzing the article formed in step (a).
Claim 18
Independent Claim
94 words
A method of preparing a ceramic article consisting essentially of silicon, carbon and nitrogen, said method comprising: (a) forming an article of the desired shape from a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; wherein the average chloride content of said polymer being less than 0.5 weight percent; and (b) pyrolyzing the article formed in step (a).
Claim 19
Dependent Claim
10 words
A ceramic article prepared by the method of claim 14.
Claim 20
Independent Claim
112 words
A method of preparing a filled ceramic article consisting essentially of silicon, carbon, nitrogen and ceramic filler, said method comprising: (a) mixing at least one ceramic filler with a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; (b) forming an article of the desired shape from said mixture of ceramic filler and methylpolydisilylazane polymer; and (c) pyrolyzing the article formed in step (b).
Claim 21
Independent Claim
112 words
A method of preparing a filled ceramic article consisting essentially of silicon, carbon, nitrogen and ceramic filler, said method comprising: (a) mixing at least one ceramic filler with a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; (b) forming an article of the desired shape from said mixture of ceramic filler and methylpolydisilylazane polymer; and (c) pyrolyzing the article formed in step (b).
Claim 22
Dependent Claim
11 words
A filled, ceramic article prepared by the method of claim 16.
Claim 23
Independent Claim
85 words
A method of preparing an article coated with a ceramic, said method comprising: (a) coating a substrate with a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; and (b) pyrolyzing the article formed in step (a).
Claim 24
Independent Claim
85 words
A method of preparing an article coated with a ceramic, said method comprising: (a) coating a substrate with a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; and (b) pyrolyzing the article formed in step (a).
Claim 25
Dependent Claim
11 words
A coated ceramic article prepared by the method of claim 18.
Claim 26
Independent Claim
99 words
A method of preparing an article coated with a ceramic, said method comprising: (a) mixing, with at least one conventional ceramic filler, a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; (b) coating a substrate with the mixture formed in (a); and (c) pyrolyzing the article formed in step (b).
Claim 27
Independent Claim
99 words
A method of preparing an article coated with a ceramic, said method comprising: (a) mixing, with at least one conventional ceramic filler, a methylpolydisilylazane polymer represented by the general formula: (Me.sub.3 SiNH).sub.6-x-2y Me.sub.x Si.sub.2 (NH).sub.y wherein the average value of x varies from 1 to 4, the average value of y varies from 1 to 2.5, and the average value of x+2y varies from 3 to 6; the average chloride content of said polymer being less than 0.5 weight percent; (b) coating a substrate with the mixture formed in (a); and (c) pyrolyzing the article formed in step (b).
Claim 28
Dependent Claim
11 words
A coated ceramic article prepared by the method of claim 20.
Claim 29
Independent Claim
78 words
A method of preparing a stable methylpolydisilylazane polymer incorporating a chloromonosilane substituted with a functional organic group, with reduced chloride content and without increased pyrophoricity, which method comprises the steps of: (a) dissolving about 15 weight percent to about 80 weight percent solids of said polymer in an organic solvent; (b) contacting the dissolved polymer with ammonia; (c) reacting the dissolved polymer with said ammonia for about 1 to about 20 hours; and (d) recovering the reacted polymer.
Claim 30
Independent Claim
78 words
A method of preparing a stable methylpolydisilylazane polymer incorporating a chloromonosilane substituted with a functional organic group, with reduced chloride content and without increased pyrophoricity, which method comprises the steps of: (a) dissolving about 15 weight percent to about 80 weight percent solids of said polymer in an organic solvent; (b) contacting the dissolved polymer with ammonia; (c) reacting the dissolved polymer with said ammonia for about 1 to about 20 hours; and (d) recovering the reacted polymer.
Claim 31
Dependent Claim
24 words
A method as recited in claim 22 wherein: said functional organic group is at least one of methylvinyl dichlorosilane, phenylvinyl dichlorosilane, and vinyl trichlorosilane.
Claim 32
Independent Claim
78 words
A method of preparing a stable methylpolydisiylyazane polymer, incorporating a chloromonosilane substituted with a nonfunctional organic group, with reduced chloride content and without increased pyrophoricity, which method comprises the steps of: (a) dissolving about 15 weight percent to about 80 weight percent solids of said polymer in an organic solvent; (b) contacting the dissolved polymer with ammonia; (c) reacting the dissolved polymer with said ammonia for about 1 to about 20 hours; and (d) recovering the reacted polymer.
Claim 33
Independent Claim
78 words
A method of preparing a stable methylpolydisiylyazane polymer, incorporating a chloromonosilane substituted with a nonfunctional organic group, with reduced chloride content and without increased pyrophoricity, which method comprises the steps of: (a) dissolving about 15 weight percent to about 80 weight percent solids of said polymer in an organic solvent; (b) contacting the dissolved polymer with ammonia; (c) reacting the dissolved polymer with said ammonia for about 1 to about 20 hours; and (d) recovering the reacted polymer.
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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) | 1991-09-20 | 1992-03-21 | 1992-09-20 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1995-09-20 | 1996-03-21 | 1996-09-20 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 1999-09-20 | 2000-03-21 | 2000-09-20 | $7700.00 | Window Closed / Lapsed |