Carbon-containing monolithic glasses prepared by a sol-gel process

Claim 1

A method of preparing a monolithic glassy ceramic which comprises drying and pyrolyzing in an inert atmosphere, or a vacuum, until a monolithic glassy ceramic is obtained, a product comprising a stable gel selected from a group consisting essentially of (A) a gel obtained from a sol of an organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH 2 =CHCH 2 -; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); (B) a gel obtained from a mixture of a sol of an organosilsesquioxane from (A),.and a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) Al 2 O 3 , (iii) ZrO 2 , (iv) TiO 2 , (v) SnO 2 , (vi) ZrSi0 4 , (vii) B 2 0 3 , (viii) La 2 O 3 and (ix) Sb 2 O 5 ; (C) a.gel obtained from a mixture of a sol of an organosilsesquioxane from (A), and a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR') wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R' is an alkyl radical of 1 to 4 carbon atoms and x has a value equivalent to the metal ion valence.

Claim 2

A method of preparing a monolithic glassy ceramic which comprises drying and pyrolyzing in an inert atmosphere, or a vacuum, until a monolithic glassy ceramic is obtained, a product comprising a stable gel selected from a group consisting essentially of (A) a gel obtained from a sol of an organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH 2 =CHCH 2 -; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); (B) a gel obtained from a mixture of a sol of an organosilsesquioxane from (A),.and a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) Al 2 O 3 , (iii) ZrO 2 , (iv) TiO 2 , (v) SnO 2 , (vi) ZrSi0 4 , (vii) B 2 0 3 , (viii) La 2 O 3 and (ix) Sb 2 O 5 ; (C) a.gel obtained from a mixture of a sol of an organosilsesquioxane from (A), and a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR') wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R' is an alkyl radical of 1 to 4 carbon atoms and x has a value equivalent to the metal ion valence.

Claim 3

A method of forming a monolithic glassy ceramic coating on a solid substrate which comprises (I) coating a solid substrate with a sol selected from a group consisting essentially of (A) a sol of organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH 2 =CHCH 2 -; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); (B) a mixture of a sol of an organosilsesquioxane from (A), and a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) Al 2 O 3 , (iii) ZrO 2 , '(iv) TiO 2 , (v) SnO 2 , (vi) ZrSiO 4 , (vii) B203, (viii) La 2 0 3 and (ix) Sb 2 O 5 ; (C) a mixture of a sol of an organosilsesquioxane from (A), and a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR') x wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R' is an alkyl - radical of 1 to 4 carbon atoms and x has a value equivalent to the metal ion valence; (II) gelling the sol while the sol is on the solid substrate; (III) drying the gel to remove volatile materials; . (IV) heat treating the gel to remove higher - boiling volatiles; and ( V ) pyrolyzing the dried and heat treated gel at a temperature of 500°C. to 1500°C, in an inert atmosphere or a vacuum until a monolithic glassy ceramic coated substrate is obtained.

Claim 4

A method of forming a monolithic glassy ceramic coating on a solid substrate which comprises (I) coating a solid substrate with a sol selected from a group consisting essentially of (A) a sol of organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH 2 =CHCH 2 -; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); (B) a mixture of a sol of an organosilsesquioxane from (A), and a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) Al 2 O 3 , (iii) ZrO 2 , '(iv) TiO 2 , (v) SnO 2 , (vi) ZrSiO 4 , (vii) B203, (viii) La 2 0 3 and (ix) Sb 2 O 5 ; (C) a mixture of a sol of an organosilsesquioxane from (A), and a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR') x wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R' is an alkyl - radical of 1 to 4 carbon atoms and x has a value equivalent to the metal ion valence; (II) gelling the sol while the sol is on the solid substrate; (III) drying the gel to remove volatile materials; . (IV) heat treating the gel to remove higher - boiling volatiles; and ( V ) pyrolyzing the dried and heat treated gel at a temperature of 500°C. to 1500°C, in an inert atmosphere or a vacuum until a monolithic glassy ceramic coated substrate is obtained.

Claim 6

A method of forming a glassy ceramic coating on a solid substrate which comprises (I) cbating a solid substrate with a stable gel selected from a group consisting essentially of (A) a gel obtained from a sol of an organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH2=CHCH2-; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); ( B ) a gel obtained from a mixture of a sol of an organosilsesquioxane from (A), and a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) Al 2 O 3 , (iii) ZrO 2 , (iv) TiO 2 , (v) Sn0 2 , (vi) ZrSiO 4 , (vii) B203, (viii) La 2 0 3 and (ix) Sb 2 O 5 ; ( C ) a gel obtained from a mixture of a sol of an organosilsesquioxane from (A), and a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR') x wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R' is an alkyl radical of 1 to 4 carbon atoms and x has a value equivalent to the metal ion valence; (II) drying the gel to remove volatile materials; (III) heat treating the gel to remove higher boiling volatiles; and (IV) pyrolyzing the dried and heat treated gel at a temperature of 500°C. to 1500°C. in an inert atmosphere or a vacuum until a monolithic glassy ceramic coated substrate is obtained.

Claim 7

A method of forming a glassy ceramic coating on a solid substrate which comprises (I) cbating a solid substrate with a stable gel selected from a group consisting essentially of (A) a gel obtained from a sol of an organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH2=CHCH2-; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); ( B ) a gel obtained from a mixture of a sol of an organosilsesquioxane from (A), and a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) Al 2 O 3 , (iii) ZrO 2 , (iv) TiO 2 , (v) Sn0 2 , (vi) ZrSiO 4 , (vii) B203, (viii) La 2 0 3 and (ix) Sb 2 O 5 ; ( C ) a gel obtained from a mixture of a sol of an organosilsesquioxane from (A), and a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR') x wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R' is an alkyl radical of 1 to 4 carbon atoms and x has a value equivalent to the metal ion valence; (II) drying the gel to remove volatile materials; (III) heat treating the gel to remove higher boiling volatiles; and (IV) pyrolyzing the dried and heat treated gel at a temperature of 500°C. to 1500°C. in an inert atmosphere or a vacuum until a monolithic glassy ceramic coated substrate is obtained.

Claim 12

A method of preparing a monolithic glassy ceramic which comprises drying and pyrolyzing in an inert atmosphere, or a vacuum, until a monolithic glassy ceramic is obtained, a product comprising a mixture of (A) a stable gel obtained from a sol of an organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH 2 =CHCH 2 -; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); (B) a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) A1 2 0 3 , (iii) ZrO 2 , (iv) TiO 2 , (v) SnO 2 , (vi) ZrSiO 4 , (vii) B 2 O 3 , (viii) La 2 O 3 and (ix) Sb 2 O 5 ; (C) a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR''') y wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R''' is an alkyl radical of 1 to 4 carbon atoms and y has a value equivalent to the metal ion valence. -

Claim 13

A method of preparing a monolithic glassy ceramic which comprises drying and pyrolyzing in an inert atmosphere, or a vacuum, until a monolithic glassy ceramic is obtained, a product comprising a mixture of (A) a stable gel obtained from a sol of an organosilsesquioxane having the unit formula RSiO 3/2 wherein R is selected from a group consisting essentially of (a) CH 2 =CH-; (b) CH 2 =CHCH 2 -; (c) C 6 H 5 -; (d) alkyl radicals of 1 to 4 carbon atoms; (e) substituted monovalent organic radicals and (f) mixtures of (a), (b), (c), (d) and (e); (B) a colloidal metal oxide or a mixture of colloidal metal oxides selected from a group consisting essentially of (i) SiO 2 , (ii) A1 2 0 3 , (iii) ZrO 2 , (iv) TiO 2 , (v) SnO 2 , (vi) ZrSiO 4 , (vii) B 2 O 3 , (viii) La 2 O 3 and (ix) Sb 2 O 5 ; (C) a metal alkoxide, or a mixture of metal alkoxides having the general formula M(OR''') y wherein M is any metal from a metal alkoxide which hydrolyzes and polymerizes in the presence of water, R''' is an alkyl radical of 1 to 4 carbon atoms and y has a value equivalent to the metal ion valence. -