Silicon carbide powder and method of preparing the same using a hydrophobic spherical silica aerogel

Patent metadata

Field	Value
Publication number	US-11220434-B2
Application number	US-201716333523-A
Country	US
Kind code	B2
Filing date	Oct 24, 2017
Priority date	May 18, 2017
Publication date	Jan 11, 2022
Grant date	Jan 11, 2022

Abstract

The present invention relates to a method of preparing ultra-pure silicon carbide in which a super-porous spherical silica aerogel is used as a silica raw material. By preparing the silica aerogel particles using low-cost water glass, a reaction area with respect to a carbon raw material is increased to enable low-temperature synthesis of silicon carbide, the size and shape of silicon carbide powder may be uniformly controlled to prepare ultra-pure silicon carbide, and economic efficiency and productivity of the silicon carbide synthesis may be improved. Thus, it is expected that the silicon carbide powder prepared by the preparation method of the present invention may be provided as an optimized raw material for the preparation of silicon carbide sintered body and single crystal (ingot).

First claim

The invention claimed is:

1. A method of preparing silicon carbide, the method comprising steps of:
(1) preparing a mixed solution comprising a carbon raw material and a silica raw material; and
(2) drying the mixed solution and heat treating the dried mixed solution in an inert atmosphere to synthesize silicon carbide,
wherein the silica raw material is a spherical silica aerogel, and wherein the spherical silica aerogel has an average particle diameter (D 50 ) of 1 μm to 1000 μm.

2. The method of claim 1 , wherein a heat treatment temperature of step (2) is in a range of 1,400° C. to 1,550° C.

3. The method of claim 2 , wherein a heat treatment temperature of step (2) is in a range of 1,525° C. to 1,550° C.

4. The method of claim 1 , wherein the spherical silica aerogel comprises a hydrophobic powder.

5. The method of claim 1 , wherein the spherical silica aerogel has a density of 0.05 g/cm 3 to 0.3 g/cm 3 .

6. The method of claim 1 , wherein the spherical silica aerogel has a specific surface area of 500 m 2 /g to 900 m 2 /g.

7. The method of claim 1 , wherein a molar ratio of the carbon raw material to the spherical silica aerogel is in a range of 0.01:1 to 100:1.

8. The method of claim 1 , wherein the inert atmosphere of step (2) comprises at least one selected from the group consisting of argon (Ar), nitrogen (N 2 ), and helium (He).

9. The method of claim 1 , further comprising a step of: (3) removing impurities.

10. The method of claim 1 , wherein the silicon carbide has an average particle diameter of 0.01 μm to 1,000 μm.

11. The method of claim 1 , wherein the spherical silica aerogel is a hydrophobic silica aerogel prepared by a preparation method including steps (a) to (f):
(a) preparing a silica precursor solution by mixing a water glass solution and a solvent, wherein the solvent does not cause a cause a change in pH of the water glass;
(b) adding a surfactant to the silica precursor solution;
(c) adding a neutralizer to the silica precursor solution after the addition of the surfactant to form a silica sol;
(d) adding a gelling agent to the silica sol to form a silica wet gel;
(e) preparing the hydrophobic silica aerogel by solvent substitution and surface modification of the silica wet gel; and
(f) drying the hydrophobic silica aerogel.

12. A method of preparing silicon carbide, the method comprising steps of:
(a) preparing a silica precursor solution by mixing a water glass solution and a solvent, wherein the solvent does not cause a change in pH of the water glass;
(b) adding a surfactant to the silica precursor solution;
(c) adding a neutralizer to the silica precursor solution after the addition of the surfactant to form a silica sol;
(d) adding a gelling agent to the silica sol to form a silica gel;
(e) preparing a hydrophobic spherical silica aerogel by solvent substitution and surface modification of the silica gel;
(f) drying the hydrophobic spherical silica aerogel;
(g) preparing a mixed solution comprising a carbon raw material and the hydrophobic spherical silica aerogel that has an average particle diameter (D 50 ) of 1 μm to 1,000 μm; and
(h) drying the mixed solution and heat treating the dried mixed solution in an inert atmosphere to synthesize silicon carbide.

13. The method of claim 12 , wherein the surfactant of step (b) comprises at least one selected from the group consisting of sorbitan monooleate, sorbitan monostearate, sorbitan monopalmitate, and sorbitan monolaurate.

14. The method of claim 12 , wherein the surfactant of step (b) is added in an amount of 3.0% to 9.0% of a total volume of the silica precursor solution.

15. The method of claim 12 , wherein the neutralizer of step (c) is added in an amount of 5% to 10% of a total volume of the silica precursor solution.

16. The method of claim 12 , wherein the gelling agent of step (d) comprises at least one selected from the group consisting of ammonia, acetone, ethanol, and isopropanol.

17. The method of claim 12 , wherein a surface modifier of step (e) is added in an amount of 5% to 20% of a total volume of the silica precursor solution.

18. The method of claim 12 , wherein a total process time of steps (a) to (f) of the preparation method is in a range of 1 hour to 5 hours.

19. The method of claim 12 , wherein the solvent is a hydrophobic non-polar organic solvent.

20. The method of claim 19 , wherein the solvent is hexane or cyclopentane.

21. The method of claim 19 , wherein the solvent substitution comprises substituting the hydrophobic non-polar organic solvent of step a) is substituted by a hydrophilic polar organic solvent.

22. The method of claim 21 , wherein the hydrophilic polar organic solvent is an alcohol-based solvent including a monovalent alcohol.

23. The method of claim 21 , wherein the hydrophilic polar organic solvent is a monovalent alcohol-based solvent having 1 to 6 carbon atoms.

24. The method of claim 12 , further comprising, after step c), stirring the silica sol at 400 rpm to 800 rpm.

Assignees

• Lg Chemical Ltd
• Univ Inha Res & Business Found

Inventors

• Kim Young Hun
• Lee Je Kyun
• Hwang Hae Jin
• Lee Kyoung Jin

Classifications

• H10D62/8325

  Silicon carbide · CPC title

• C01B32/97 Primary

  Preparation from SiO or SiO2 · CPC title

• C01B33/1585

  Dehydration into aerogels · CPC title

• C01P2006/10

  Solid density · CPC title

• C01B33/158

  Purification; Drying; Dehydrating · CPC title