Compound transparent ceramics and methods of preparation thereof

• US 8,329,090 B2
• Filed: 10/21/2009
• Issued: 12/11/2012
• Est. Priority Date: 10/24/2008
• Status: Active Grant

• Current Assignee: Lawrence Livermore National Security LLC (Government of the United States of America)
• Original Assignee: Lawrence Livermore National Security LLC (Government of the United States of America)
• Inventors: Hollingsworth, Joel P., Kuntz, Joshua D., Soules, Thomas F., Landingham, Richard L.
• Primary Examiner(s): WIESE, NOAH S
• Application Number:
  US12/603,195
• Publication Number:
  US 20100105539A1
• Time in Patent Office: 1,147 Days
• Field of Search: 501/152, 501/153, 264/681, 264/621, 264/642, 264/653
• US Class Current: 264/642
• CPC Class Codes: B32B 18/00 Layered products essentially comprising ceramics, e.g. refractory products
• CPC Class Codes: B82Y 30/00 Nanotechnology for materials or surface science, e.g. nanocomposites
• CPC Class Codes: C04B 2235/3224 Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
• CPC Class Codes: C04B 2235/3225 Yttrium oxide or oxide-forming salts thereof
• CPC Class Codes: C04B 2235/5454 nanometer sized, i.e. below 100 nm
• CPC Class Codes: C04B 2235/549 the particle size being expressed by crystallite size or primary particle size
• CPC Class Codes: C04B 2235/9653 Translucent or transparent ceramics other than alumina
• CPC Class Codes: C04B 2237/58 Forming a gradient in composition or in properties across the laminate or the joined articles
• CPC Class Codes: C04B 35/44 based on aluminates
• CPC Class Codes: C04B 35/6263 characterised by their solids loadings, i.e. the percentage of solids
• CPC Class Codes: C04B 35/6264 Mixing media, e.g. organic solvents
• CPC Class Codes: C04B 35/62665 Flame, plasma or melting treatment
• CPC Class Codes: C04B 35/6269 Curing of mixtures

Abstract

According to one embodiment, a method for forming a composite transparent ceramic preform includes forming a first suspension of oxide particles in a first solvent which includes a first dispersant but does not include a gelling agent, adding the first suspension to a first mold of a desired shape, and uniformly curing the first suspension in the first mold until stable. The method also includes forming a second suspension of oxide particles in a second solvent which includes a second dispersant but does not include a gelling agent, adding the second suspension to the stable first suspension in a second mold of a desired shape encompassing the first suspension and the second suspension, and uniformly curing the second suspension in the second mold until stable. Other methods for forming a composite transparent ceramic preform are also described according to several other embodiments. Structures are also disclosed.

Claims

1. A method for forming a composite transparent ceramic preform, the method comprising:

forming a first suspension of oxide particles in a first solvent, wherein the first suspension includes a first dispersant, with the proviso that the first suspension does not include a gelling agent;

adding the first suspension to a first mold of a desired shape;

uniformly curing the first suspension in the first mold until stable;

forming a second suspension of oxide particles in a second solvent, wherein the second suspension includes a second dispersant, with the proviso that the second suspension does not include a gelling agent;

adding the second suspension to the stable first suspension in a second mold of a desired shape encompassing the first suspension and the second suspension;

uniformly curing the second suspension in the second mold until stable.

2. The method of claim 1, wherein the oxide particles have a primary particle diameter of between about 5 nm and about 2000 nm.

10. The method of claim 1, wherein the curing the first suspension and the second suspension comprises:

heating the first suspension in the first mold and the second suspension in the second mold to a temperature of between about 20°

C. and about 80°

C.; and

holding the temperature about constant for a time of between about 4 hours and about 72 hours.

11. The method of claim 10, wherein the first mold and the second mold are sealed during the curing, and wherein the first suspension and the second suspension are heated to a temperature of about 50°

C.

13. The method of claim 10, further comprising calcining the cured second suspension at a temperature of between about 500°

C. and about 1100°

C.

14. The method of claim 1, wherein the first suspension has an active dopant, wherein the second suspension has an active dopant different from the active dopant of the first suspension or wherein the second suspension has a different concentration of the same active dopant as the active dopant of the first suspension.

15. The method of claim 1, wherein the first and second solvents comprise at least one of:

water, ammonia, nitric acid, yttrium nitrate, aluminum nitrate, an alcohol, an aldehyde, an organic solvent, and urea.

16. The method of claim 1, wherein the first and second dispersants comprise at least one of:

an ammonium polymethacrylate, a narrow molecular weight range ammonium polyacrylate, a free metal ion salt, sodium silicate, and ammonium acrylate.

19. The method of claim 1, wherein the stable first and second suspensions are

a graded and/or composite preform, the preform being mechanically stable without support,

wherein the oxide particles in the preform are unsintered inorganic particles.

20. The method of claim 19, wherein creating the preform includes a gel casting process.

21. The method of claim 19, wherein the creating the preform comprises:

adding a first mixture of the inorganic particles and a solvent to a first mold;

adding a second mixture of inorganic particles and a solvent to a second mold where the second mixture abuts the first and second molds; and

removing the molds prior to curing the first and second mixtures.

22. The method of claim 19, wherein the creating the preform comprises:

adding a first mixture of the inorganic particles and a solvent to a first mold;

at least partially curing the first mixture; and

adding a second mixture of inorganic particles and a solvent to a second mold, where the second mixture abuts the first and second molds after the adding.

23. The method of claim 19, wherein the creating the preform comprises:

forming a first preform in a mold;

removing the mold from the first preform; and

forming a second preform around the first preform in a second mold.

24. The method of claim 19, wherein the creating the preform comprises:

adding a mixture of the inorganic particles and a solvent to a mold;

allowing the mixture to gel; and

injecting a dopant into a target region of the gelled mixture.

25. The method of claim 19, wherein the creating the preform comprises:

adding a mixture comprising the inorganic particles and a solvent to a mold;

allowing the mixture to gel;

exchanging liquid in the gelled mixture with a solution having a dopant; and

adding a second mixture of inorganic particles in contact with the gelled mixture, wherein some of the dopant diffuses into the second mixture.

26. The method of claim 19, wherein the preform is transparent after sintering thereof.

27. The method of claim 19, wherein the preform includes a first portion comprising neodymium doped yttrium aluminum garnet (Nd:

YAG) and a second portion immediately adjacent the first portion comprising samariam doped yttrium aluminum garnet (Sm;

YAG).

28. The method of claim 1, further comprising calcining the cured first suspension at a temperature of between about 500°

C. and about 1100°

C.

29. The method of claim 1, further comprising calcining the cured second suspension at a temperature of between about 500°

C. and about 1100°

C.

30. The method of claim 1, wherein the second suspension is added to the stable first suspension prior to sintering the stable first suspension.

31. The method of claim 1, wherein the second suspension is added to the stable first suspension prior to calcining the stable first suspension.

32. The method of claim 1, wherein the second suspension is added to the stable first suspension prior to drying the stable first suspension.

33. The method of claim 1, wherein the curing the first suspension continues without drying until the preform is removed from the second mold.

34. The method of claim 1, wherein the first mold and the second mold are sealed during the curing.

3. A method for forming a composite transparent ceramic preform, the method comprising:

forming a first suspension of oxide particles in a first solvent, wherein the first suspension includes a first dispersant, with the proviso that the first suspension does not include a gelling agent;

adding the first suspension to a first mold of a desired shape;

uniformly curing the first suspension in the first mold until stable;

forming a second suspension of oxide particles in a second solvent, wherein the second suspension includes a second dispersant, with the proviso that the second suspension does not include a gelling agent;

adding the second suspension to the stable first suspension in a second mold of a desired shape encompassing the first suspension and the second suspension; and

uniformly curing the second suspension in the second mold until stable.

wherein the oxide particles have a primary particle diameter of between about 10 nm and about 80 nm.

4. The method of claim 3, wherein the oxide particles are formed via flame-spray pyrolysis (FSP).

5. The method of claim 4, wherein the oxide particles comprise at least one of yttrium aluminum garnet (YAG), neodymium doped YAG, yttrium scandium aluminum garnet, lutetium aluminum garnet, gadolinium gallium garnet, yttrium oxide, ytterbium doped yttrium oxide, doped scaudia, doped lutetia, and doped zirconia.

6. The method of claim 4, wherein the first and second solvents have a pH of between about 2 and about 5 or between about 9 and about 12.

7. The method of claim 6, wherein a volume percent of solids in a total volume of the first and second suspensions is between about 15 vol. % and about 60 vol. %.

8. The method of claim 6, wherein a volume percent of solids in a total volume of the first and second suspensions is between about 25 vol. % and about 45 vol. %.

9. The method of claim 4, wherein the oxide particles comprise YAG, wherein the first and second solvents have a pH of between about 9 and about 11, wherein a volume percent of solids in a total volume of the first and second suspensions is between about 25 vol. % and about 45 vol. %.

12. A method for forming a composite transparent ceramic preform, the method comprising:

forming a first suspension of oxide particles in a first solvent, wherein the first suspension includes a first dispersant, with the proviso that the first suspension does not include a gelling agent;

adding the first suspension to a first mold of a desired shape;

uniformly curing the first suspension in the first mold until stable;

forming a second suspension of oxide particles in a second solvent, wherein the second suspension includes a second dispersant, with the proviso that the second suspension does not include a gelling agent;

adding the second suspension to the stable first suspension in a second mold of a desired shape encompassing the first suspension, and the second suspension;

uniformly curing the second suspension in the second mold until stable;

wherein the curing the first suspension and the second suspension comprises;

heating the first suspension in the first mold and the second suspension in the second mold to a temperature of between about 20°

C. and about 80°

C., and

holding the temperature about constant for a time of between about 4 hours and about 72 hours; and

calcining at least one of the cured first suspension and the cured second suspension at a temperature of between about 500°

C. and about 1100°

C.

17. A method, comprising:

forming a first suspension of oxide particles in a first solvent, wherein the first suspension includes a first dispersant, with the proviso that the first suspension does not include a gelling agent;

agitating the first suspension;

adding the first suspension to a first mold of a desired shape;

uniformly drying the first suspension in the first mold until stable;

forming a second suspension of oxide particles in a second solvent, wherein the second suspension includes a second dispersant, with the proviso that the second suspension does not include a gelling agent;

agitating the second suspension;

adding the second suspension to the stable first suspension in a second mold of a desired shape encompassing the first suspension and the second suspension;

curing the first suspension and the second suspension in the second mold at a temperature of between about 20°

C. and about 80°

C. until stable.

18. The method of claim 17, further comprising sintering the cured suspensions for forming a composite transparent ceramic.

35. The method of claim 17, wherein the oxide particles have a primary particle diameter of between about 10 nm and about 80 nm.

36. The method of claim 17, further comprising calcining at least one of the cured first suspension and the cured second suspension at a temperature of between about 500°

C. and about 1100°

C.

37. The method of claim 17, wherein the second mold is sealed during the curing.