US4898842A
Expired / Lapsed
US
⏱️ 0.0 years remaining
Organometallic-derived cordierite and other compounds comprising oxides of silicon
Assignee: International Business Machines Corp
•
Filing: 1987-09-14
•
Granted: 1990-02-06
•
Expires: 2007-09-14
Abstract
Abstract The present invention provides a method of synthesizing amorphous cordierite-forming glasses from organometallic precursors. Either the sol-gel/β-diketonate technique or the amorphous chelating hydroxycarboxylate process can be used advantageously. The method of the present invention can also be used to form 5 component comprised and 2 component comprised amorphous compositions wherein one of the components is an oxide of silicon.
Inventors
- 👤 Lawrence D. David
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-10-30 21:37
CPC Classifications
C; C03; C03C; C03C10/00; C03C10/0036; C03C10/0045
Claims Analysis
Total Claims: 36
Claim 1
Independent Claim
121 words
A method of producing amorphous powders comprising cordierite-forming glasses, wherein the method comprises: (a) forming an aqueous or organic solution having an aqueous or organic solvent, respectively, and containing at least two precursors of said amorphous powders comprising cordierite, wherein said precursors are β-diketonates of magnesium and aluminum or chelating hydroxycarboxylates of aluminum and magnesium; (b) adding to said solution a silane; (c) adding to said solution a reagent capable of hydrolyzing at least said silane wherein said precursor components, said silane, and said hydrolyzing reagent undergo a polymerization reaction; (d) stripping from said aqueous or organic solution the aqueous or organic solvent, leaving a residue; (e) pyrolyzing said residue to produce a fine, amorphous powder comprised of amorphous cordierite-forming glass.
Claim 2
Independent Claim
121 words
A method of producing amorphous powders comprising cordierite-forming glasses, wherein the method comprises: (a) forming an aqueous or organic solution having an aqueous or organic solvent, respectively, and containing at least two precursors of said amorphous powders comprising cordierite, wherein said precursors are β-diketonates of magnesium and aluminum or chelating hydroxycarboxylates of aluminum and magnesium; (b) adding to said solution a silane; (c) adding to said solution a reagent capable of hydrolyzing at least said silane wherein said precursor components, said silane, and said hydrolyzing reagent undergo a polymerization reaction; (d) stripping from said aqueous or organic solution the aqueous or organic solvent, leaving a residue; (e) pyrolyzing said residue to produce a fine, amorphous powder comprised of amorphous cordierite-forming glass.
Claim 3
Dependent Claim
29 words
The method of claim 1 wherein said solution is organic and said precursors of said cordierite-forming glasses are comprised of a β-diketonate of magnesium, and a β-diketonate of aluminum.
Claim 4
Dependent Claim
61 words
The method of claim 2 wherein said β-diketonates are of the general structure ##STR2## wherein M is magnesium or aluminum and n is 2 for magnesium or 3 for aluminum, and wherein R=CH 3 , alkyl, aryl, or CF 3 ; R'=CH 3 , alkyl, aryl, or CF 3 , and R"=H, CH 3 , alkyl, aryl or CF 3 .
Claim 5
Dependent Claim
15 words
The method of claim 2 or claim 3 wherein said organic solution solvent is water-miscible.
Claim 6
Dependent Claim
28 words
The method of claim 4 wherein said organic solution solvent is selected from the group consisting of tetrahydrofuran, ethanol, methanol, glycol ethers, dimethylsulfoxide, dimethylformamide, dimethylacetamide, and mixtures thereof.
Claim 7
Dependent Claim
26 words
The method of claim 1 wherein said solution is aqueous and said precursors of said cordierite-forming glasses are comprised of chelating hydroxycarboxylates of aluminum and magnesium.
Claim 8
Dependent Claim
25 words
The method of claim 6 wherein said chelating hydroxycarboxylate is selected from the group consisting of citrates, maleates, tartrates, lactates and esters of glycolic acid.
Claim 9
Dependent Claim
43 words
The method of claim 5 wherein said silane is selected from the group consisting of alkoxysilanes of the general formula Si (OR) 4 , wherein R is any alkyl or aryl group, and wherein the alkoxysilane is soluble in said organic solution solvent.
Claim 10
Dependent Claim
10 words
The method of claim 8 wherein said silane is tetraethoxysilane.
Claim 11
Dependent Claim
39 words
The method of claim 8 wherein said hydrolyzing reagent is comprised of a dilute acid selected from the group consisting of HNO 3 , HCl, HBr, HI, HF, CH 3 COOH, H 2 SO 4 , and sulfonic acids.
Claim 12
Dependent Claim
17 words
The method of claim 2, wherein said solvent is stripped from said solution using spray drying techniques.
Claim 13
Dependent Claim
23 words
The method of claim 8, wherein said solvent of said solvent or water of said aqueous solution is stripped using spray drying techniques.
Claim 14
Dependent Claim
51 words
The method of claim 12, wherein said pyrolyzing is carried out in two steps comprising: heating said gel in an inert atmosphere to a temperature as high as about 500° C., followed by heating the resultant partially pyrolyzed material in an oxidizing atmosphere to a temperature as high as 700° C.
Claim 15
Dependent Claim
23 words
The method of claim 12 wherein said pyrolyzing is carried out in an oxidizing atmosphere to a temperature as high as 700° C.
Claim 16
Dependent Claim
30 words
The method of claim 8 wherein combinations of phosphorous and boron oxides are introduced into said cordierite-comprising powders by using phosphoric acid and aqueous boric acid as said hydrolyzing reagents.
Claim 17
Dependent Claim
55 words
The method of claim 8 wherein combinations of phosphorus oxides and boron oxides are introduced into said cordierite-forming glass comprising powders by adding phosphorous alkoxides to said organic or said aqueous solution, hydrolyzing said organic or said aqueous solution containing said phosphorous alkoxides, and then adding boron alkoxides to said organic or said aqueous solution.
Claim 18
Dependent Claim
25 words
The method of claim 1 wherein said solution is aqueous and said precursors of said cordierite components are comprised of magnesium citrate and aluminum citrate.
Claim 19
Dependent Claim
43 words
The method of claim 17 wherein said silane is selected from the group consisting of alkoxy silanes of the general formula Si(OR) 4 , wherein R is any alkyl or aryl group which permits said silane to remain soluble in said aqueous solution.
Claim 20
Dependent Claim
10 words
The method of claim 18 wherein said silane is tetraethoxysilane.
Claim 21
Dependent Claim
13 words
The method of claim 19 wherein said hydrolyzing reagent is a dilute acid.
Claim 22
Dependent Claim
21 words
The method of claim 17 or claim 20, wherein said aqueous solvent is stripped from said solution using spray drying techniques.
Claim 23
Dependent Claim
22 words
The method of claim 21 wherein said pyrolyzing is carried out in an oxidizing atmosphere to temperatures as high as 700° C.
Claim 24
Dependent Claim
31 words
The method of claim 17 wherein combinations of phosphorous oxides and boron oxides are introduced into said cordierite-forming glass comprising composition by using phosphoric acid and aqueous boric acid hydrolyzing reagents.
Claim 25
Dependent Claim
45 words
The method of claim 17 wherein combinations of phosphorous oxides and boron oxides are introduced into said cordierite-forming glass comprising composition by adding phosphorous alkoxides to said aqueous solution, hydrolyzing said phosphorous alkoxide containing aqueous solution, and then adding boron alkoxides to said aqueous solution.
Claim 26
Independent Claim
149 words
A method of producing a glassy, amorphous powder comprising two components, wherein one of said two components is an oxide of silicon, wherein the method comprises: (a) forming an aqueous or organic solution having an aqueous or organic solvent, respectively, and containing one non-silicon-containing precursor of said amorphous composition, wherein said precursor is a β-diketonate of magnesium, aluminum or boron or a citrate of magnesium or aluminum; (b) adding to said solution a silane; (c) adding to said solution a reagent capable of hydrolyzing said silane wherein said non-silicon-containing precursor component, said silane, and said hydrolyzing reagent undergo a polymerization reaction; (d) stripping from said aqueous or organic solution the aqueous or organic solvent using spray drying techniques, leaving a residue; (e) pyrolyzing said residue to produce a fine, amorphous powder comprised of a two component amorphous composition wherein one of said two components is an oxide of silicon.
Claim 27
Independent Claim
149 words
A method of producing a glassy, amorphous powder comprising two components, wherein one of said two components is an oxide of silicon, wherein the method comprises: (a) forming an aqueous or organic solution having an aqueous or organic solvent, respectively, and containing one non-silicon-containing precursor of said amorphous composition, wherein said precursor is a β-diketonate of magnesium, aluminum or boron or a citrate of magnesium or aluminum; (b) adding to said solution a silane; (c) adding to said solution a reagent capable of hydrolyzing said silane wherein said non-silicon-containing precursor component, said silane, and said hydrolyzing reagent undergo a polymerization reaction; (d) stripping from said aqueous or organic solution the aqueous or organic solvent using spray drying techniques, leaving a residue; (e) pyrolyzing said residue to produce a fine, amorphous powder comprised of a two component amorphous composition wherein one of said two components is an oxide of silicon.
Claim 28
Dependent Claim
75 words
The method of claim 25 wherein said solution is organic and said one non-silicon-containing precursor is comprised of a β-diketonate of the general structure ##STR3## wherein M is magnesium or aluminum or boron, and n is a number equal to the valence of M, and wherein R=CH 3 , alkyl, aryl, or CF 3 ; R'=CH 3 , alkyl, aryl, or CF 3 ; and R"=H, CH 3 , alkyl, aryl, or CF 3 .
Claim 29
Dependent Claim
14 words
The method of claim 25 or claim 26 wherein said organic solvent is water-miscible.
Claim 30
Dependent Claim
31 words
The method of claim 25 wherein said solution is aqueous and said one non-silicon-containing precursor is comprised of a citrate selected from the group consisting of magnesium citrate and aluminum citrate.
Claim 31
Dependent Claim
52 words
Amorphous cordierite-forming powders comprising two major components, wherein one of said two major components is an oxide of magnesium, aluminum, boron, phosphorus or mixtures thereof and wherein the particles are equiaxed and the mean particle size ranges from about 50Å to about 80Å which upon sintering, followed by crystallization, will produce cordierite.
Claim 32
Dependent Claim
52 words
Amorphous cordierite-forming powders comprising two major components, wherein one of said two major components is an oxide of magnesium, aluminum, boron, phosphorus or mixtures thereof and wherein the particles are equiaxed and the mean particle size ranges from about 50Å to about 80Å which upon sintering, followed by crystallization, will produce cordierite.
Claim 33
Dependent Claim
29 words
The amorphous powders of claim 29 wherein said about 50Å to about 80Å particles are soft agglomarated into agglomerates ranging from about 800Å to about 5 micrometers in size.
Claim 34
Dependent Claim
29 words
The amorphous, cordierite-forming powders of claim 29 wherein said about 50Å to about 80Å particles are soft agglomerated into agglomerates ranging from about 800Å to about 1000Å in size.
Claim 35
Dependent Claim
16 words
Amorphous cordierite-forming powders of claim 29 which upon sintering, followed by crystallization, will form μ-phase cordierite.
Claim 36
Dependent Claim
24 words
Amorphous cordierite-forming powders of claim 29 which comprises boron oxides and phosphorous oxides, and which upon sintering, followed by crystallization, will form α-phase cordierite.
References Cited (Backward Citations)
US3640093A
Cited
US4028085A
Cited
US4217240A
Cited
US4234367A
Cited
US4301132A
Cited
US4340436A
Cited
JPS5788075A
Cited
US4486401A
Cited
US4473542A
Cited
US4698317A
Cited
US4764486A
Cited
USPTO Annuity & Maintenance Windows
| Annuity Stage | Window Opens | Payment Deadline | Surcharge Period Until | Estimated Fee | Status |
|---|---|---|---|---|---|
| 3.5 Years (Year 4) | 1993-02-05 | 1993-08-07 | 1994-02-06 | $2000.00 | Window Closed / Lapsed |
| 7.5 Years (Year 8) | 1997-02-05 | 1997-08-07 | 1998-02-06 | $3760.00 | Window Closed / Lapsed |
| 11.5 Years (Year 12) | 2001-02-05 | 2001-08-07 | 2002-02-06 | $7700.00 | Window Closed / Lapsed |