US5272239A
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Silicon-filled aluminum polymer precursors to SiC-AlN ceramics
Assignee: Clariant Finance BVI Ltd
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Filing: 1992-03-24
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Granted: 1993-12-21
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Expires: 2012-03-24
Abstract
Abstract Process for producing ceramic compositions by dispersing elemental silicon powder in a ceramic precursor polymer containing Al, N, and C, shaping the resultant composition, and heating the shaped product to cause a reaction between the elemental silicon and the polymer to result in an intermediate composition and further heating the intermediate composition to a temperature sufficient to consolidate the char to a dense SiC--AlN solid-solution or microscopic ceramic.
Inventors
- 👤 James A. Jensen
Bibliographic Details
Application Number
—
Jurisdiction
US
Data Source
google_patents
Last Synchronized
2026-11-03 13:07
CPC Classifications
C; C04; C04B; C04B35/00; C04B35/515; C04B35/58; C04B35/581; C04B35/56; C04B35/565; C04B35/571; C04B35/573
Claims Analysis
Total Claims: 36
Claim 1
Independent Claim
388 words
A process for preparing a composition, said process comprising: reacting a composition comprising a mixture of elemental silicon and a polymer comprising aluminum, nitrogen, and carbon in an atmosphere at a temperature sufficient to form a refractory reaction product comprising silicon-carbon bonds and aluminum-nitrogen bonds, wherein said polymer comprising aluminum, nitrogen and carbon has a general formula selected from the group of formulae consisting of: ##STR9## where n>2 and R and R"' can be the same or different and are selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R', R" and R"' are not all hydrogen; ##STR10## where n>2 and R is an imine group, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R' and R" are not all hydrogen; ##STR11## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, and aryloxy groups; and ##STR12## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups and hydrogen provided that R and R' are not both hydrogen and x+y<1, and in the group containing y repeat units the aluminum atom is bonded to three nitrogen atoms.
Claim 2
Dependent Claim
388 words
A process for preparing a composition, said process comprising: reacting a composition comprising a mixture of elemental silicon and a polymer comprising aluminum, nitrogen, and carbon in an atmosphere at a temperature sufficient to form a refractory reaction product comprising silicon-carbon bonds and aluminum-nitrogen bonds, wherein said polymer comprising aluminum, nitrogen and carbon has a general formula selected from the group of formulae consisting of: ##STR9## where n>2 and R and R"' can be the same or different and are selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R', R" and R"' are not all hydrogen; ##STR10## where n>2 and R is an imine group, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R' and R" are not all hydrogen; ##STR11## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, and aryloxy groups; and ##STR12## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups and hydrogen provided that R and R' are not both hydrogen and x+y<1, and in the group containing y repeat units the aluminum atom is bonded to three nitrogen atoms.
Claim 3
Dependent Claim
12 words
The process of claim 1, wherein said elemental silicon is silicon powder.
Claim 4
Dependent Claim
116 words
The process of claim 1 wherein said polymer comprising aluminum, nitrogen and carbon has the general formula: ##STR13## wherein n≧2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen provided that R and R' are not both hydrogen and x+y≦1, and in the group containing y repeat units the aluminum atom is bonded to three nitrogen atoms.
Claim 5
Dependent Claim
26 words
The process of claim 1, wherein said alkyl groups are selected from the group consisting of methyl, ethyl, isopropyl, butyl, isobutyl, pentyl, hexyl, and heptyl groups.
Claim 6
Dependent Claim
28 words
The process of claim 1, wherein said cycloalkenyl groups are selected from the group consisting of organounsaturated groups which are capable of being crosslinked by an energy input.
Claim 7
Dependent Claim
28 words
The process of claim 1, wherein said alkenyl groups are selected from the group consisting of organounsaturated groups which are capable of being crosslinked by an energy input.
Claim 8
Dependent Claim
23 words
The process of claim 6, wherein said organounsaturated groups are selected from the group consisting of allyl, methallyl, butenyl, 2-methylpropenyl, and propenyl groups.
Claim 9
Dependent Claim
12 words
The process of claim 1, wherein said atmosphere is a nonoxidizing atmosphere.
Claim 10
Dependent Claim
23 words
The process of claim 8, wherein said nonoxidizing atmosphere is selected from the group consisting of an argon-containing atmosphere, and a nitrogen-containing atmosphere.
Claim 11
Dependent Claim
18 words
The process of claim 1, wherein said reaction temperature is a temperature of up to about 1650° C.
Claim 12
Dependent Claim
20 words
The process of claim 10, wherein said reaction temperature is a temperature between about 400° C. and about 1650° C.
Claim 13
Dependent Claim
26 words
The process of claim 1, wherein said refractory reaction product comprising silicon carbon bonds and aluminum-nitrogen bonds comprises a mixture of silicon carbide and aluminum nitride.
Claim 14
Dependent Claim
23 words
The process of claim 12, wherein said mixture of silicon carbide and aluminum nitride comprises a mixture of beta-silicon carbide and aluminum nitride.
Claim 15
Dependent Claim
32 words
The process of claim 1, further comprising heating said refractory reaction product in an atmosphere at a temperature sufficient to sinter said refractory reaction product and form a sintered refractory reaction product.
Claim 16
Dependent Claim
12 words
The process of claim 14, wherein said atmosphere is a nonoxidizing atmosphere.
Claim 17
Dependent Claim
23 words
The process of claim 15, wherein said nonoxidizing atmosphere is selected from the group consisting of an argon-containing atmosphere and a nitrogen-containing atmosphere.
Claim 18
Dependent Claim
22 words
The process of claim 14, wherein said temperature sufficient to sinter is a temperature between about 1650° C. and about 2200° C.
Claim 19
Dependent Claim
22 words
The process of claim 17, wherein said temperature sufficient to sinter is a temperature between about 1900° C. and about 2200° C.
Claim 20
Dependent Claim
21 words
The process of claim 14, wherein said sintered refractory reaction product comprises a sintered composite of alpha-silicon carbide and aluminum nitride.
Claim 21
Dependent Claim
24 words
The process of claim 19, wherein said sintered composite of alpha-silicon carbide and aluminum nitride comprises a microcomposite of alpha-silicon carbide and aluminum nitride.
Claim 22
Dependent Claim
21 words
The process of claim 14, wherein said sintered refractory reaction product comprises a solid solution of alpha-silicon carbide and aluminum nitride.
Claim 23
Dependent Claim
28 words
The process of claim 1, wherein said composition comprises a sufficient excess of said elemental silicon to result in said refractory reaction product which contains unreacted elemental silicon.
Claim 24
Dependent Claim
43 words
The process of claim 22, wherein said refractory reaction product is heated in an atmosphere comprising a member selected from the group consisting of ammonia and nitrogen and mixtures thereof to provide a ternary ceramic comprising silicon carbide, aluminum nitride, and silicon nitride.
Claim 25
Dependent Claim
358 words
A composition comprising a mixture of elemental silicon and a polymer comprising aluminum, nitrogen and carbon, wherein said polymer comprising aluminum, nitrogen and carbon has a general formula selected from the group of formulae consisting of: wherein n>2 and R and R"' can be the same or different and are selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R', R" and R"' are not all hydrogen; ##STR14## wherein n>2 and R is an imine group, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R' and R" are not all hydrogen; ##STR15## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, and aryloxy groups; and ##STR16## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups and hydrogen provided that R and R' are not both hydrogen and x+y<1, and in the group containing y repeat units the aluminum atom is bonded to three nitrogen atoms.
Claim 26
Dependent Claim
358 words
A composition comprising a mixture of elemental silicon and a polymer comprising aluminum, nitrogen and carbon, wherein said polymer comprising aluminum, nitrogen and carbon has a general formula selected from the group of formulae consisting of: wherein n>2 and R and R"' can be the same or different and are selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R', R" and R"' are not all hydrogen; ##STR14## wherein n>2 and R is an imine group, and R' and R" may be selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen, provided that R, R' and R" are not all hydrogen; ##STR15## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, and aryloxy groups; and ##STR16## where n>2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups and hydrogen provided that R and R' are not both hydrogen and x+y<1, and in the group containing y repeat units the aluminum atom is bonded to three nitrogen atoms.
Claim 27
Dependent Claim
116 words
The process of claim 24 wherein said polymer comprising aluminum, nitrogen and carbon has the general formula: ##STR17## where n≧2 and R is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, and hydrogen, and R' is selected from the group consisting of 1-12 carbon alkyl groups, 3-12 carbon cycloalkyl groups, 2-12 carbon alkenyl groups, 3-12 carbon cycloalkenyl groups, aryl groups, amino groups, imino groups, carboxy groups, alkoxy groups, aryloxy groups, and hydrogen provided that R and R' are not both hydrogen and x+y≦1, and in the group containing y repeat units the aluminum atom is bonded to three nitrogen atoms.
Claim 28
Dependent Claim
27 words
The composition of claim 24, wherein said alkyl groups are selected from the group consisting of methyl, ethyl, propyl, isopropyl, butyl, isobutyl, pentyl, hexyl, and heptyl groups.
Claim 29
Dependent Claim
28 words
The composition of claim 24, wherein said alkenyl groups are selected from the group consisting of organounsaturated groups which are capable of being crosslinked by an energy input.
Claim 30
Dependent Claim
28 words
The composition of claim 24, wherein said cycloalkenyl groups are selected from the group consisting of organounsaturated groups which are capable of being crosslinked by an energy input.
Claim 31
Dependent Claim
22 words
The composition of claim 28, wherein said organo-unsaturated groups are selected from the group consisting of allyl, butenyl, 2-methylpropenyl, and propenyl groups.
Claim 32
Dependent Claim
9 words
The composition of claim 24, further comprising a filler.
Claim 33
Dependent Claim
24 words
The composition of claim 30, wherein said filler comprises a member selected from the group consisting of alpha-silicon carbide, beta-silicon carbide, and mixtures thereof.
Claim 34
Dependent Claim
11 words
The composition of claim 30, wherein said filler comprises aluminum nitride.
Claim 35
Dependent Claim
12 words
The composition of claim 30, wherein said filler comprises a sintering aid.
Claim 36
Dependent Claim
25 words
The composition of claim 33, wherein said sintering aid comprises a member selected from the group consisting of yttrium oxide, calcium oxide, and aluminum oxide.
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