Claims
- 1. A process for forming a high purity material consisting essentially of silicon, nitrogen, and hydrogen by the reaction of particulate elemental silicon with a nitrogen-hydrogen reactant in its liquid state at a low reaction temperature which comprises:
- (a) removing surface coatings on said particulate elemental silicon to promote reaction between said silicon and said nitrogen-hydrogen reactant; and
- (b) reacting said particulate elemental silicon at a temperature, equivalent at atmospheric temperature, of under about 200.degree. C. with a nitrogen-hydrogen reactant having the formula:
- N.sub.n H.sub.(n+m)
- wherein: n=1-4; and m=2 when the nitrogen-hydrogen reactant is a straight chain, and 0 when the nitrogen-hydrogen reactant is cyclic.
- 2. The process of claim 1 wherein said surface coatings on said elemental silicon particulate are removed by chemical treatment of said silicon with a reagent capable of removing said coating.
- 3. The process of claim 1 wherein said surface coatings on said elemental silicon particulate are removed by heating said particulate to a temperature of at least 1300.degree. C. in a reducing atmosphere.
- 4. The process of claim 1 wherein said surface coatings on said elemental particulate silicon are removed by milling said particulate silicon during said reaction of said particulate silicon with said N.sub.n H.sub.(n+m) reactant.
- 5. The process of claim 1 wherein said elemental silicon has a purity of 99.9 wt.% or greater when n=1 and 95 wt.% or greater when n=2-4.
- 6. The process of claim 1 wherein said elemental silicon has a purity of at least 99.9 wt.%.
- 7. The process of claim 6 wherein said particulate elemental silicon has a purity of at least 99.999 wt.%.
- 8. The process of claim 1 wherein said particulate elemental silicon used in said reaction has a particle size range of from about 0.01 microns to about 100 mesh (Tyler).
- 9. The process of claim 8 wherein said particulate elemental silicon used in said reaction has a particle size range of from about 0.01 microns to about 150 microns.
- 10. The process of claim 1 wherein said N.sub.n H.sub.(n+m) reactant comprises a compound having a boiling point, equivalent at atmospheric pressure, of under 200.degree. C.
- 11. The process of claim 10 wherein said N.sub.n H.sub.(n+m) reactant is selected from the class consisting of ammonia; a hydrazine having the formula N.sub.n H.sub.(n+2) where n=2-4; a cyclic hydrazine having the formula N.sub.n H.sub.n, where n=3-4; and mixtures thereof.
- 12. The process of claim 11 wherein said N.sub.n H.sub.(n+m) reactant consists essentially of ammonia and said reaction temperature range is a temperature, equivalent at atmospheric pressure, of from about -40.degree. C. to about -125.degree. C.
- 13. The process of claim 11 wherein said N.sub.n H.sub.(n+m) reactant consists essentially of hydrazine (N.sub.2 H.sub.4) and said reaction temperature range is a temperature, equivalent at atmospheric pressure, of from about 0.degree. C. to about 100.degree. C.
- 14. The process of claim 1 wherein said low reaction temperature ranges from about 15.degree. C. to about 100.degree. C. below the boiling point of said N.sub.n H.sub.(n+m) reactant.
- 15. The process of claim 1 wherein said N.sub.n H.sub.(n+m) reactant is present in stoichiometric excess with respect to said elemental silicon reactant.
- 16. The process of claim 1 wherein said elemental silicon is reacted with said N.sub.n H.sub.(n+m) reactant for a period of from about less than 1 hour up to about 100 hours.
- 17. The process of claim 16 wherein said reaction time is from about 30 minutes up to about 50 hours.
- 18. The process of claim 1 wherein said process is run on a continuous basis and said reactants have a contact time together of from less than 1 hour up to about 100 hours.
- 19. The process of claim 1 including the further step of heating said reaction product to a temperature of from about 1200.degree.-1700.degree. C. in a nonreactive atmosphere to convert said reaction product to a crystalline material consisting essentially of alpha silicon nitride.
- 20. A process for producing, at a temperature, equivalent at atmospheric temperature, to not more than about 100.degree. C., a high purity reaction product consisting essentially of silicon, nitrogen, and hydrogen which comprises: reacting together elemental particulate silicon having a particle size range of from about 0.01 to 150 microns and a purity of at least about 99.9 wt.% with a reactive nitrogen-hydrogen liquid having the formula:
- N.sub.n H.sub.(n+m)
- wherein:
- n=1-4 and
- m=2 for a straight chain configuration; or
- m=0 for a cyclic configuration;
- while simultaneously milling said elemental particulate silicon during said reaction of said silicon with said N.sub.n H.sub.(n+m) reactant to reduce the particle size of said silicon particulate, to accelerate the reaction time by exposing fresh surfaces of said silicon particulate for reaction with said N.sub.n H.sub.(n+m) reactant, and to remove surface coatings on said particulate elemental silicon.
- 21. A process for continuously producing a high purity reaction product consisting essentially of silicon, nitrogen, and hydrogen from particulate metallic silicon and a reactive nitrogen-hydrogen liquid which comprises:
- (a) milling in a reaction vessel elemental silicon particles having a purity of at least 99.9 wt.%, at a temperature, equivalent at atmospheric pressure, of under 200.degree. C. in the presence of a reactive nitrogen-hydrogen liquid selected from the class consisting of ammonia; a hydrazine having the formula N.sub.n H.sub.(n+2) where n=2-4; a cyclic hydrazine having the formula N.sub.n H.sub.n, where n=3-4; and mixtures thereof to cause said reactive nitrogen-hydrogen liquid to react with the exposed surfaces of the milled elemental silicon particles to form an intermediate reaction product;
- (b) continuously removing liquid from said reaction vessel containing an intermediate product consisting essentially of silicon, nitrogen, and hydrogen; and
- (c) recovering a solid intermediate product from said liquid containing said intermediate product.
- 22. A process for producing, at a low reaction temperature, a high purity silicon nitride from particulate elemental silicon and a nitrogen-hydrogen reactant in its liquid state which comprises:
- (a) removing surface coatings on said particulate elemental silicon to promote reaction between said silicon and said nitrogen-hydrogen reactant;
- (b) reacting together, at a temperature, equivalent at atmospheric pressure, of less than 200.degree. C., a particulate elemental silicon having a particle size range of from about 0.01 to 150 microns and a purity of at least about 99.9 wt.% and a nitrogen-hydrogen reactant in its liquid state having the formula: N.sub.n H.sub.(n+m) wherein: n=1-4, and m=2 when the nitrogen-hydrogen reactant is straight chain and 0 when the nitrogen-hydrogen reactant is cyclic, to form an intermediate reaction product; and
- (c) heating said intermediate reaction product to a temperature of from about 1200.degree.-1700.degree. C. in a nonreactive atmosphere to convert said intermediate reaction product to a crystalline material consisting essentially of alpha silicon nitride.
- 23. A process for continuously producing high purity silicon nitride from particulate metallic silicon and a reactive nitrogen-hydrogen liquid which comprises:
- (a) milling in a reaction vessel elemental silicon particles having a purity of at least 99.9 wt.%, at a temperature, equivalent at atmospheric pressure, of under 200.degree. C. in the presence of a reactive nitrogen-hydrogen liquid selected from the class consisting of ammonia; a hydrazine having the formula N.sub.n H.sub.(n+2) where n=2-4; a cyclic hydrazine having the formula N.sub.n H.sub.n, where n=3-4; and mixtures thereof to cause said reactive nitrogen-hydrogen liquid to react with the exposed surfaces of the milled elemental silicon particles to form an intermediate reaction product;
- (b) continuously removing liquid from said reaction vessel containing said intermediate reaction product consisting essentially of silicon, nitrogen, and hydrogen;
- (c) recovering a solid intermediate product from said liquid containing said intermediate product; and
- (d) heating said intermediate product at a temperature of from about 1200.degree.-1700.degree. C. for a period of from about 15 minutes up to about 2 hours to convert said intermediate product to high purity alpha silicon nitride.
Parent Case Info
This is a continuation of application Ser. No. 096,577, filed Sep. 15, 1987, now abandoned.
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Continuations (1)
|
Number |
Date |
Country |
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96527 |
Sep 1987 |
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