Process of synthesizing mixed BaO-TiO.sub.2 based powders for ceramic applications

• US 4,606,906 A
• Filed: 11/15/1984
• Issued: 08/19/1986
• Est. Priority Date: 11/15/1984
• Status: Expired due to Fees

• Current Assignee: THE GOVERNMENT OF THE UNITED STATES OF AMERICA, AS REPRESENTED BY THE SECRETARY OF COMMERCE
• Original Assignee: THE GOVERNMENT OF THE UNITED STATES OF AMERICA, AS REPRESENTED BY THE SECRETARY OF COMMERCE
• Inventors: Negas, Taki, Ritter, Joseph J., Roth, Robert S.
• Primary Examiner(s): Dixon, Jr., William R.
• Assistant Examiner(s): Group, Karl
• Application Number:
  US06/671,539
• Time in Patent Office: 642 Days
• Field of Search: 501/137, 501/12, 501/138, 501/136, 423/598
• US Class Current: 423/598
• CPC Class Codes: C01G 23/006 Alkaline earth titanates
• CPC Class Codes: C01P 2002/02 Amorphous compounds
• CPC Class Codes: C01P 2006/36 Solid to solid transition temperatures
• CPC Class Codes: C04B 35/4686 based on phases other than BaTiO3 perovskite phase

Abstract

A process for producing any desired Ba/Ti mixture to be formulated as an amorphous solid which crystallizes at very low temperatures to yield a desired phase or phases is disclosed. The process yields products free of undesirable impurities and allows macroscopic production of certain phases in the baria-titania system, having exceptional high frequency dielectric properties, that were previously unattainable through solid-state high temperature production techniques.

Claims

1. A process for synthesizing single phase crystalline Ba₂ Ti₉ O₂₀ powders comprising the steps of:

(a) dissolving barium oxide in a first lower alkyl alcohol in a dry atmosphere to form a barium alkoxide solution;

(b) dissolving a titanium alkoxide in a second lower alkyl alcohol in a dry atmosphere to form a titanium alkoxide solution;

(c) combining said barium alkoxide solution and said titanium alkoxide solution in a dry atmosphere to form a mixed barium-titanium alkoxide system wherein the molar ratio of barium to titanium in said mixed system is approximately 2;

9;

(d) subjecting said mixed barium-titanium alkoxide system to hydrolysis at a reflux temperature of between 70°

C. and 90°

C. to form a precipitate;

(e) separating said precipitate and drying said precipitate; and

(f) heating said precipitate at a temperature of between 700°

C. and 1100°

C. for approximately between 15-20 hours to form a crystalline, single phase of Ba₂ Ti₉ O₂₀.

2. The process of claim 1, wherein said mixed barium-titanium alkoxide system is subjected to hydrolysis by adding an ethanol-water solution to said system.

3. The process of claim 2, wherein said ethanol-water solution contains water in a 10 to 20% excess over that required to hydrolyze all alkoxy groups of said mixed barium-titanium alkoxide solution.

4. The process of claim 1, wherein said titanium alkoxide is titanium isopropoxide.

5. The process of claim 1, wherein said first lower alkyl alcohol and said second lower alkyl alcohol have from 1 to 3 carbon atoms.

6. The process of claim 1, wherein said first lower alkyl alcohol and said second lower alkyl alcohol are ethanol.

7. A process for synthesizing single phase crystalline Ba₂ Ti₉ O₂₀ powders comprising the steps of:

(a) dissolving barium oxide in a first lower alkyl alcohol in a dry atmosphere to form a barium alkoxide solution;

(b) dissolving a titanium alkoxide in a second lower alkyl alcohol in a dry atmosphere to form a titanium alkoxide solution;

(c) combining said barium alkoxide solution and said titanium alkoxide solution to form a mixed barium-titanium alkoxide system wherein the molar ratio of barium to titanium in said mixed system is approximately 2;

9;

(d) stirring said mixed barium-titanium alkoxide system to form a precipitate;

(e) subjecting said mixed barium-titanium alkoxide system containing said precipitate to hydrolysis at a reflux temperature of between 70°

C. and 90°

C.;

(f) separating said precipitate and drying said precipitate; and

(g) heating said precipitate at a temperature of between 700°

C. and 1100°

C. for between 15 and 20 hours to form a crystalline, single phase of Ba₂ Ti₉ O₂₀.

8. The process of claim 7, wherein said mixed barium-titanium alkoxide system containing said precipitate is subjected to hydrolysis by adding an ethanol-water solution to said system.

9. The process of claim 8, wherein said ethanol-water solution contains water in a 10 to 20% excess over that required to hydrolyze all alkoxy groups of said mixed barium-titanium alkoxide solution.

10. The process of claim 7, wherein said titanium alkoxide is titanium isopropoxide.

11. The process of claim 7, wherein said first lower alkyl alcohol and said second lower alkyl alcohol have from 1 to 3 carbon atoms.

12. The process of claim 7, wherein said first lower alkyl alcohol and second lower alkyl alcohol are ethanol.

13. A process for synthesizing single phase crystalline BaTi₅ O₁₁ powders comprising the steps of:

(a) dissolving barium oxide in a first lower alkyl alcohol to form a barium alkoxide solution;

(b) dissolving a titanium alkoxide in a second lower alkyl alcohol to form a titanium alkoxide solution;

(c) combining said barium alkoxide solution and said titanium alkoxide solution to form a mixed barium-titanium alkoxide system wherein the molar ratio of barium to titanium in said mixed system is approximately one to five;

(d) stirring said mixed barium-titanium alkoxide system to form a first precipitate;

(e) heating said mixed barium-titanium alkoxide system containing said first precipitate at a reflux temperature of between 70°

C. and 90°

C. for between 15-20 hours to dissolve said first precipitate and form a second precipitate;

(f) subjecting said mixed barium-titanium alkoxide system containing said second precipitate to hydrolysis to form a precursor;

(g) separating and drying said second precipitate; and

(h) calcining said precipitate at between 700°

C. and 1100°

C. for a period of between 15 and 20 hours to form a crystalline, single phase of BaTi₅ O₁₁.

14. The process of claim 13, wherein said mixed barium-titanium alkoxide system containing said second precipitate is subjected to hydrolysis by adding an ethanol-water solution to said system.

15. The process of claim 13, wherein said ethanol-water solution contains water in a 10 to 20% excess over that required to hydrolyze all alkoxy groups of said mixed barium-titanium alkoxide solution.

16. The process of claim 13, wherein said titanium alkoxide is titanium isopropoxide.

17. The process of claim 13, wherein said first lower alkyl alcohol and said second lower alkyl alcohol have from 1 to 3 carbon atoms.

18. The process of claim 13, wherein said first lower alkyl alcohol and said second lower alkyl alcohol are ethanol.