US20020016248A1 - Reaction synthesis of silicon carbide-boron nitride composites - Google Patents
Reaction synthesis of silicon carbide-boron nitride composites Download PDFInfo
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- US20020016248A1 US20020016248A1 US09/747,939 US74793900A US2002016248A1 US 20020016248 A1 US20020016248 A1 US 20020016248A1 US 74793900 A US74793900 A US 74793900A US 2002016248 A1 US2002016248 A1 US 2002016248A1
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- silicon carbide
- boron nitride
- silicon
- boron
- nitride
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- 239000010703 silicon Substances 0.000 title claims abstract description 63
- 229910052710 silicon Inorganic materials 0.000 title claims abstract description 63
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 title claims abstract description 53
- 238000006243 chemical reaction Methods 0.000 title claims abstract description 41
- 230000015572 biosynthetic process Effects 0.000 title 1
- 238000003786 synthesis reaction Methods 0.000 title 1
- 229910052582 BN Inorganic materials 0.000 claims abstract description 95
- 239000002131 composite material Substances 0.000 claims abstract description 67
- 239000000203 mixture Substances 0.000 claims abstract description 50
- 229910052581 Si3N4 Inorganic materials 0.000 claims abstract description 46
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims abstract description 45
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims abstract description 44
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims abstract description 44
- 229910010271 silicon carbide Inorganic materials 0.000 claims abstract description 43
- 239000000843 powder Substances 0.000 claims abstract description 42
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 40
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 39
- 229910052580 B4C Inorganic materials 0.000 claims abstract description 36
- INAHAJYZKVIDIZ-UHFFFAOYSA-N boron carbide Chemical compound B12B3B4C32B41 INAHAJYZKVIDIZ-UHFFFAOYSA-N 0.000 claims abstract description 35
- 238000011065 in-situ storage Methods 0.000 claims abstract description 35
- 239000002245 particle Substances 0.000 claims abstract description 18
- 238000000465 moulding Methods 0.000 claims abstract description 15
- 238000005245 sintering Methods 0.000 claims abstract description 15
- 239000011159 matrix material Substances 0.000 claims abstract description 10
- 238000000034 method Methods 0.000 claims description 21
- 238000004519 manufacturing process Methods 0.000 claims description 20
- 239000000463 material Substances 0.000 description 18
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 13
- RUDFQVOCFDJEEF-UHFFFAOYSA-N yttrium(III) oxide Inorganic materials [O-2].[O-2].[O-2].[Y+3].[Y+3] RUDFQVOCFDJEEF-UHFFFAOYSA-N 0.000 description 11
- 229910052593 corundum Inorganic materials 0.000 description 10
- 229910001845 yogo sapphire Inorganic materials 0.000 description 10
- 238000007731 hot pressing Methods 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 3
- 230000007797 corrosion Effects 0.000 description 3
- 238000005260 corrosion Methods 0.000 description 3
- 238000013001 point bending Methods 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 230000035939 shock Effects 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 2
- 238000005452 bending Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000003779 heat-resistant material Substances 0.000 description 2
- 238000010297 mechanical methods and process Methods 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- -1 ytterbia Chemical compound 0.000 description 2
- 229910017083 AlN Inorganic materials 0.000 description 1
- PIGFYZPCRLYGLF-UHFFFAOYSA-N Aluminum nitride Chemical compound [Al]#N PIGFYZPCRLYGLF-UHFFFAOYSA-N 0.000 description 1
- 241000968352 Scandia <hydrozoan> Species 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000003466 anti-cipated effect Effects 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 1
- 230000001747 exhibiting effect Effects 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- HJGMWXTVGKLUAQ-UHFFFAOYSA-N oxygen(2-);scandium(3+) Chemical compound [O-2].[O-2].[O-2].[Sc+3].[Sc+3] HJGMWXTVGKLUAQ-UHFFFAOYSA-N 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/56—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides
- C04B35/565—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide
- C04B35/573—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide obtained by reaction sintering or recrystallisation
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/58—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides
- C04B35/583—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides based on boron nitride
Definitions
- the present invention relates to a silicon carbide-boron nitride composite material comprising silicon carbide-boron nitride or silicon carbide-silicon nitride-boron nitride, obtained through an in-situ chemical reaction of same, and to a method for the manufacture of same, and in particular relates to the manufacturing and thereby providing of silicon carbide-boron nitride composite materials in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix, by utilising an in-situ chemical reaction between silicon nitride, boron carbide and carbon.
- the present invention relates to a novel material which displays exceptional strength and corrosion resistance and which has a low elastic modulus and provides a material which can be utilised in such diverse applications as thermal shock resistant materials, mechanical shock resistant materials, heat resistant materials or corrosion resistant materials.
- silicon carbide is known as a sinter material containing silicon nitride, aluminium nitride, boron nitride and titanium boride as additives, as disclosed in U.S. Pat. No. 4,304,870, for example.
- Silicon carbide-boron nitride composite materials have conventionally been manufactured by mixing presynthesised silicon carbide and boron nitride powder using a mechanical method, then hot-pressing etc. the resulting mixture. With this method, however, the coarser the boron nitride powder is, the coarser the boron nitride particles will be in the resulting composite material. Due to boron nitride exhibiting a high anisotropy of thermal expansion, cracks tend to form along boundary surfaces; therefore, the larger the particles are, the less strength the composite materials will have.
- boron nitride powder is preferable due to it being a fine powder; however, such fine powders are expensive and moreover it is difficult to eliminate the coarse powder completely.
- the present invention relates to a silicon carbide-boron nitride composite material, which synthesised according to an in-situ chemical reaction between silicon nitride, boron carbide and carbon, and which contains fine boron nitride particles dispersed in a silicon carbide matrix, wherein aforementioned composite material is obtained by molding a powder mixture containing each of the components required in the in-situ reaction and sintering the mixture; and is a method for manufacturing the aforementioned material, wherein aforementioned method for manufacturing the silicon carbide-boron nitride composite material comprises molding a powder in which each component which is required in the in-situ chemical reaction between silicon carbide, boron nitride and carbon is admixed, and, as required, at least one component selected from among silicon carbide, boron nitride or silicon nitride is further added thereinto and the mixture is sintered to obtain the composite.
- the present invention in resolving the aforementioned drawbacks, comprises the technical means below.
- said silicon carbide-boron nitride composite material is produced by molding a powder mixture containing the said components which are required in the in-situ chemical reaction, and sintering the molded mixture to obtain the sintered composite.
- a silicon carbide-boron nitride composite material which synthesised according to an in-situ chemical reaction between at least silicon nitride, boron carbide and carbon,
- said silicon carbide-boron nitride composite material is produced by molding a powder comprising a silicon carbide, boron nitride or silicon nitride powder being added to a powder mixture containing the said components which are required in the in-situ chemical reaction between silicon nitride, boron carbide and carbon, and sintering the molded mixture to obtain the sintered composite comprising silicon carbide-boron nitride or silicon carbide-silicon nitride-boron nitride in which the phase composition is adjusted as required.
- a silicon carbide-boron nitride composite material which synthesised according to an in-situ chemical reaction between at least silicon nitride, boron carbide and carbon,
- said silicon carbide-boron nitride composite material is produced by molding a powder comprising a silicon carbide or boron nitride powder being added to a powder mixture containing the said components which are required in an in-situ chemical reaction between silicon nitride, boron carbide and carbon, and sintering the molded mixture to obtain the sintered composite in which the phase composition is adjusted as required.
- a method for manufacturing the composite material defined in any one of (1) through (3) above which comprises mixing the components which are required in an in-situ chemical reaction between silicon nitride, boron carbide and carbon, adding further as required, at least one component selected from among silicon carbide, boron nitride or silicon nitride thereinto, molding the mixture, and sintering the molded mixture to manufacture a silicon carbide-boron nitride composite material or a silicon carbide-silicon nitride-boron nitride composite material.
- a silicon carbide-boron nitride composite material in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix, by means of an in-situ chemical reaction between silicon nitride, boron carbide and carbon, is manufactured and thereby provided.
- the uniform dispersing of the fine boron nitride particles by means of an in-situ chemical reaction of same enables fracture toughness to be enhanced, while significantly lowering the elastic modulus, without causing the strength of the resulting silicon carbide-boron nitride composite material to diminish.
- silicon carbide-boron nitride composite materials can be manufactured with the present invention according to the following chemical reaction:
- the composite material synthesised according to the in-situ chemical reaction between silicon nitride, boron carbide and carbon shall be defined to be a composite material that has been synthesised according to the aforesaid chemical reaction.
- the phase composition obtained from this chemical reaction is 46.29 vol % silicon carbide and 53.71 vol % boron nitride. If the amount of silicon nitride added in such circumstances is greater than the stoichiometric composition; i.e., is added in excess, a silicon carbide-silicon nitride-boron nitride composite material shall be obtained. In the present invention, it is possible to produce silicon carbide-silicon nitride-boron nitride composite materials by adding an amount of silicon nitride which is in excess of the stoichiometric composition of the aforesaid chemical reaction.
- a silicon carbide-boron nitride composite material in which the phase composition has been adjusted to the required level can be manufactured by further adding silicon carbide or boron nitride powder to a powder mixture containing each component in the aforesaid chemical reaction.
- a silicon carbide-silicon nitride-boron nitride composite material with the desired phase composition can be manufactured by further adding a silicon carbide, boron nitride or silicon nitride powder.
- each component required in the in-situ chemical reaction between silicon nitride, boron carbide and carbon are mixed, whereupon the mixture is moulded and sintered; however, it is possible to manufacture silicon carbide-boron nitride composite materials or silicon carbide-silicon nitride-boron nitride composite materials, in which the phase composition has been adjusted as required, by moulding and sintering a powder that contains at least one component selected from among silicon carbide, boron nitride or silicon nitride, and that has been added, as required, to the powder mixture containing each component.
- an ⁇ -type silicon nitride powder of a mean particle diameter of 0.5 ⁇ to be used as the silicon nitride in the material for e.g. a boron carbide powder of a mean particle diameter of 1 ⁇ to be used as the boron carbide; for e.g. an ⁇ -type silicon carbide powder of a mean particle diameter of 0.6 ⁇ to be used as the silicon carbide; and for e.g. a carbon powder of a mean particle diameter of 0.01 ⁇ to be used as the carbon; however, the invention is not limited to the above.
- These materials can be mixed into a powder mixture using a ball mill.
- Hot-pressing can be used to mould and sinter the powder mixture into the desired form.
- the hot-pressing is preferably carried out under a pressure of 10 to 50 MPa in an inert gas atmosphere of e.g. argon gas, preferably utilising e.g., the in-situ chemical reaction between silicon nitride, boron carbide and carbon.
- alumina, yttria, magnesia, ytterbia, zirconia, silica, lutetia, ceria, scandia or another sintering auxiliary can be preferably added to yield a fine composite material containing no air pockets.
- a silicon carbide-boron nitride composite material is synthesised by moulding and sintering a powder mixture containing each component, utilising the in-situ chemical reaction between silicon nitride, boron carbide and carbon; accordingly, using an uncomplicated process it is possible to manufacture a silicon carbide-boron nitride composite material, in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix.
- silicon carbide-boron nitride composite materials have been manufactured by mixing pre-synthesised silicon carbide and boron nitride powders by means of a mechanical method and then e.g., hot-pressing the mixture.
- the coarser the boron nitride powder is the coarser the boron nitride particles will be in the resulting composite materials, and the less strength the composite materials will have.
- fine boron nitride powder is expensive and moreover it is technically difficult to eliminate the coarse powder completely.
- the method pertaining to the present invention which utilises an in-situ chemical reaction between silicon nitride, boron carbide and carbon, it is possible to manufacture a silicon carbide-boron nitride composite material with an uncomplicated process, in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix. Therefore, fracture toughness can be enhanced and the elastic modulus significantly lowered, without causing the strength of the silicon carbide-boron nitride composite material to diminish. It is therefore possible to manufacture silicon carbide-boron nitride composites which exhibit high performance, inexpensively.
- the materials used for the present invention and for comparative examples were manufactured by mixing powders containing each of the aforesaid raw material components, then applying a known moulding and sintering method, such as hot-pressing, to the resulting mixtures.
- a known moulding and sintering method such as hot-pressing
- B55 in Table 1 approximately 60 wt % silicon nitride, 24 wt % boron carbide, 10 wt % carbon, 4 wt % alumina and 2 wt % yttria were mixed together, and the resulting mixture was hot-pressed for one hour at 2000° C. to yield a fine material free of air pockets.
- the strength, elastic moduli and fracture toughness values of the materials were respectively assessed using a three-point bending strength testing method in accordance with JIS R1601, an ultrasonic pulse method in accordance with JIS R1602 and an IF method in accordance with JIS R1607.
- the results of the measurements were a three-point bending strength of approximately 350 MPa, an elastic modulus of 107 GPa and a fracture toughness value of 6.7 MPam 1 ⁇ 2 .
- This working example is represented as B55 in Table 1, and the other working examples are also represented in Table 1, all having been tested using the same methods as described above.
- TABLE 1-1 Phase composition of Hot-pressing Bending Elastic Fracture Sample Composition of raw resulting material temperature strength modulus toughness No.
- B0, carbon 55 and carbon 25 are given in Table 1 as comparative examples.
- the hot-pressed sintered articles produced from silicon carbide-boron nitride powder mixtures displayed a three-point bending strength of approximately 250 MPa and a fracture toughness of 5 MPam 1 ⁇ 2 , which were recognised as coming substantially below the values for all of the working examples.
- the present invention relates to a silicon carbide-boron nitride composite material, which is obtained in accordance with an in-situ chemical reaction between silicon nitride, boron carbide and carbon, by moulding and sintering a powdered mixture containing each component, and a method for the manufacture of same.
- the following exceptional merits can be obtained: 1) it is possible to manufacture and thereby to provide a silicon carbide-boron nitride composite material in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix; 2) using an uncomplicated process it is possible to obtain a silicon carbide-boron nitride composite material which exhibits high strength, a low elastic modulus, and high fracture toughness at room temperature, by utilising an in-situ chemical reaction between silicon nitride, boron carbide and carbon, mixing each component powder together and then hot-pressing the mixture; and 3) it is possible to manufacture a silicon carbide-boron nitride composite material of high performance, inexpensively.
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Abstract
The present invention relates to a silicon carbide-boron nitride composite material, which synthesised according to an in-situ chemical reaction between silicon nitride, boron carbide and carbon, and which contains fine boron nitride particles dispersed in a silicon carbide matrix, wherein aforementioned composite material is obtained by molding a powder mixture containing each of the components required in the in-situ reaction and sintering the mixture.
Description
- 1. Field of the Invention
- The present invention relates to a silicon carbide-boron nitride composite material comprising silicon carbide-boron nitride or silicon carbide-silicon nitride-boron nitride, obtained through an in-situ chemical reaction of same, and to a method for the manufacture of same, and in particular relates to the manufacturing and thereby providing of silicon carbide-boron nitride composite materials in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix, by utilising an in-situ chemical reaction between silicon nitride, boron carbide and carbon.
- The present invention relates to a novel material which displays exceptional strength and corrosion resistance and which has a low elastic modulus and provides a material which can be utilised in such diverse applications as thermal shock resistant materials, mechanical shock resistant materials, heat resistant materials or corrosion resistant materials.
- 2. Description of the Related Art
- Due to its exceptional resistance to oxidation and heat, silicon carbide is known as a sinter material containing silicon nitride, aluminium nitride, boron nitride and titanium boride as additives, as disclosed in U.S. Pat. No. 4,304,870, for example.
- Due to their exceptional resistance to oxidation and corrosion, these materials are used as heat-resistant materials in air furnaces, and it is expected that as their properties are enhanced, their range of application will accordingly expand. The addition of boron nitride in particular allows the thermal shock resistance of the resulting composite material to be significantly enhanced, leading to anticipated applications in such fields as aircraft engine or gas turbine components.
- Silicon carbide-boron nitride composite materials have conventionally been manufactured by mixing presynthesised silicon carbide and boron nitride powder using a mechanical method, then hot-pressing etc. the resulting mixture. With this method, however, the coarser the boron nitride powder is, the coarser the boron nitride particles will be in the resulting composite material. Due to boron nitride exhibiting a high anisotropy of thermal expansion, cracks tend to form along boundary surfaces; therefore, the larger the particles are, the less strength the composite materials will have.
- Accordingly, boron nitride powder is preferable due to it being a fine powder; however, such fine powders are expensive and moreover it is difficult to eliminate the coarse powder completely.
- With the foregoing problems with the prior art in view, the inventors of the present invention attempted to develop a new composite material, and a method for the manufacture of same, with which it is possible to eliminate completely the drawbacks with the aforementioned method, and having conducted diligent research in regard to the manufacture of composite ceramic materials utilising an in-situ chemical reaction discovered that silicon carbide-boron nitride composite materials can be manufactured by utilising an in-situ chemical reaction between silicon nitride, boron carbide and carbon and conducting a hot-press process on a powder mixture containing silicon nitride, boron carbide and carbon, involving a controlled rate of temperature increase. The inventors further discovered that an even finer material could be manufactured, which contained no air pockets, by further adding a sinter auxiliary such as alumina or yttria, and perfected the present invention based on these findings.
- It is an object of the present invention to provide, by utilising a simple in-situ chemical reaction, a method for manufacturing a silicon carbide-boron nitride composite material, and the composite material itself, which when compared with composites manufactured using traditional methods exhibits a finer structure, higher density, higher strength, lower elastic modulus and higher fracture toughness. The present invention relates to a silicon carbide-boron nitride composite material, which synthesised according to an in-situ chemical reaction between silicon nitride, boron carbide and carbon, and which contains fine boron nitride particles dispersed in a silicon carbide matrix, wherein aforementioned composite material is obtained by molding a powder mixture containing each of the components required in the in-situ reaction and sintering the mixture; and is a method for manufacturing the aforementioned material, wherein aforementioned method for manufacturing the silicon carbide-boron nitride composite material comprises molding a powder in which each component which is required in the in-situ chemical reaction between silicon carbide, boron nitride and carbon is admixed, and, as required, at least one component selected from among silicon carbide, boron nitride or silicon nitride is further added thereinto and the mixture is sintered to obtain the composite.
- It is an object of the present invention to manufacture, and thereby to provide, a silicon carbide-boron nitride composite material in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix, by means of an in-situ chemical reaction.
- It is a further object of the present invention to manufacture, and thereby to provide, a silicon carbide-silicon nitride-boron nitride composite material by utilising an in-situ chemical reaction between silicon nitride, boron carbide and carbon.
- The present invention, in resolving the aforementioned drawbacks, comprises the technical means below.
- (1) A silicon carbide-boron nitride composite material with fine boron nitride particles uniformly dispersed in a silicon carbide matrix, which synthesised according to an in-situ chemical reaction between silicon nitride, boron carbide and carbon,
- said silicon carbide-boron nitride composite material is produced by molding a powder mixture containing the said components which are required in the in-situ chemical reaction, and sintering the molded mixture to obtain the sintered composite.
- (2) A silicon carbide-boron nitride composite material, which synthesised according to an in-situ chemical reaction between at least silicon nitride, boron carbide and carbon,
- said silicon carbide-boron nitride composite material is produced by molding a powder comprising a silicon carbide, boron nitride or silicon nitride powder being added to a powder mixture containing the said components which are required in the in-situ chemical reaction between silicon nitride, boron carbide and carbon, and sintering the molded mixture to obtain the sintered composite comprising silicon carbide-boron nitride or silicon carbide-silicon nitride-boron nitride in which the phase composition is adjusted as required.
- (3) A silicon carbide-boron nitride composite material, which synthesised according to an in-situ chemical reaction between at least silicon nitride, boron carbide and carbon,
- said silicon carbide-boron nitride composite material is produced by molding a powder comprising a silicon carbide or boron nitride powder being added to a powder mixture containing the said components which are required in an in-situ chemical reaction between silicon nitride, boron carbide and carbon, and sintering the molded mixture to obtain the sintered composite in which the phase composition is adjusted as required.
- (4) A method for manufacturing the composite material defined in any one of (1) through (3) above, which comprises mixing the components which are required in an in-situ chemical reaction between silicon nitride, boron carbide and carbon, adding further as required, at least one component selected from among silicon carbide, boron nitride or silicon nitride thereinto, molding the mixture, and sintering the molded mixture to manufacture a silicon carbide-boron nitride composite material or a silicon carbide-silicon nitride-boron nitride composite material.
- The present invention shall now be described in further detail.
- According to the present invention, as has been detailed in the foregoing, a silicon carbide-boron nitride composite material, in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix, by means of an in-situ chemical reaction between silicon nitride, boron carbide and carbon, is manufactured and thereby provided.
- In the present invention, in other words, the uniform dispersing of the fine boron nitride particles by means of an in-situ chemical reaction of same enables fracture toughness to be enhanced, while significantly lowering the elastic modulus, without causing the strength of the resulting silicon carbide-boron nitride composite material to diminish.
- To provide a more detailed explanation, silicon carbide-boron nitride composite materials can be manufactured with the present invention according to the following chemical reaction:
- Si3N4+B4C+2C=3SiC+4BN
- In the present invention, the composite material synthesised according to the in-situ chemical reaction between silicon nitride, boron carbide and carbon shall be defined to be a composite material that has been synthesised according to the aforesaid chemical reaction.
- The phase composition obtained from this chemical reaction is 46.29 vol % silicon carbide and 53.71 vol % boron nitride. If the amount of silicon nitride added in such circumstances is greater than the stoichiometric composition; i.e., is added in excess, a silicon carbide-silicon nitride-boron nitride composite material shall be obtained. In the present invention, it is possible to produce silicon carbide-silicon nitride-boron nitride composite materials by adding an amount of silicon nitride which is in excess of the stoichiometric composition of the aforesaid chemical reaction.
- A silicon carbide-boron nitride composite material in which the phase composition has been adjusted to the required level can be manufactured by further adding silicon carbide or boron nitride powder to a powder mixture containing each component in the aforesaid chemical reaction. Moreover, a silicon carbide-silicon nitride-boron nitride composite material with the desired phase composition can be manufactured by further adding a silicon carbide, boron nitride or silicon nitride powder.
- In the present invention, essentially, each component required in the in-situ chemical reaction between silicon nitride, boron carbide and carbon are mixed, whereupon the mixture is moulded and sintered; however, it is possible to manufacture silicon carbide-boron nitride composite materials or silicon carbide-silicon nitride-boron nitride composite materials, in which the phase composition has been adjusted as required, by moulding and sintering a powder that contains at least one component selected from among silicon carbide, boron nitride or silicon nitride, and that has been added, as required, to the powder mixture containing each component.
- In the present invention, it is preferable for e.g. an α-type silicon nitride powder of a mean particle diameter of 0.5μ to be used as the silicon nitride in the material; for e.g. a boron carbide powder of a mean particle diameter of 1μ to be used as the boron carbide; for e.g. an α-type silicon carbide powder of a mean particle diameter of 0.6μ to be used as the silicon carbide; and for e.g. a carbon powder of a mean particle diameter of 0.01μ to be used as the carbon; however, the invention is not limited to the above. These materials can be mixed into a powder mixture using a ball mill. Hot-pressing can be used to mould and sinter the powder mixture into the desired form. The hot-pressing is preferably carried out under a pressure of 10 to 50 MPa in an inert gas atmosphere of e.g. argon gas, preferably utilising e.g., the in-situ chemical reaction between silicon nitride, boron carbide and carbon.
- In conducting the above, alumina, yttria, magnesia, ytterbia, zirconia, silica, lutetia, ceria, scandia or another sintering auxiliary can be preferably added to yield a fine composite material containing no air pockets.
- In the present invention, a silicon carbide-boron nitride composite material is synthesised by moulding and sintering a powder mixture containing each component, utilising the in-situ chemical reaction between silicon nitride, boron carbide and carbon; accordingly, using an uncomplicated process it is possible to manufacture a silicon carbide-boron nitride composite material, in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix.
- (Function)
- In the past, silicon carbide-boron nitride composite materials have been manufactured by mixing pre-synthesised silicon carbide and boron nitride powders by means of a mechanical method and then e.g., hot-pressing the mixture. However, the coarser the boron nitride powder is, the coarser the boron nitride particles will be in the resulting composite materials, and the less strength the composite materials will have. On the other hand, fine boron nitride powder is expensive and moreover it is technically difficult to eliminate the coarse powder completely.
- According to the method pertaining to the present invention, which utilises an in-situ chemical reaction between silicon nitride, boron carbide and carbon, it is possible to manufacture a silicon carbide-boron nitride composite material with an uncomplicated process, in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix. Therefore, fracture toughness can be enhanced and the elastic modulus significantly lowered, without causing the strength of the silicon carbide-boron nitride composite material to diminish. It is therefore possible to manufacture silicon carbide-boron nitride composites which exhibit high performance, inexpensively.
- The present invention shall be described in further detail with reference to working examples. The present invention shall in no way be limited to these examples.
- (1) Composition of Raw Material
- Tests in the present working examples were conducted on powders containing each of the raw material components as given in Table 1.
- (2) Method
- The materials used for the present invention and for comparative examples were manufactured by mixing powders containing each of the aforesaid raw material components, then applying a known moulding and sintering method, such as hot-pressing, to the resulting mixtures. Taking B55 in Table 1 as an example, approximately 60 wt % silicon nitride, 24 wt % boron carbide, 10 wt % carbon, 4 wt % alumina and 2 wt % yttria were mixed together, and the resulting mixture was hot-pressed for one hour at 2000° C. to yield a fine material free of air pockets.
- (3) Results
- The strength, elastic moduli and fracture toughness values of the materials were respectively assessed using a three-point bending strength testing method in accordance with JIS R1601, an ultrasonic pulse method in accordance with JIS R1602 and an IF method in accordance with JIS R1607. The results of the measurements were a three-point bending strength of approximately 350 MPa, an elastic modulus of 107 GPa and a fracture toughness value of 6.7 MPam ½. This working example is represented as B55 in Table 1, and the other working examples are also represented in Table 1, all having been tested using the same methods as described above.
TABLE 1-1 Phase composition of Hot-pressing Bending Elastic Fracture Sample Composition of raw resulting material temperature strength modulus toughness No. material (wt %) (vol %) (° C.) (MPa) (GPa) (MPam½) B0 90 silicon carbide 100 silicon carbide 2000 620 427 4 7 Al2O3 3 Y2O3 B5 83.1 silicon carbide 95 silicon carbide 2000 675 370 — 4.6 silicon nitride 5 boron nitride 1.8 boron carbide 0.8 carbon 6.8 Al2O3 2.9 Y2O3 B15 68.6 silicon carbide 85 silicon carbide 2000 647 295 — 14.3 silicon nitride 15 boron nitride 5.7 boron carbide 2.5 carbon 6.3 Al2O3 2.7 Y2O3 B25 53.3 silicon carbide 75 silicon carbide 2000 588 240 6.7 25.1 silicon nitride 25 boron nitride 9.9 boron carbide 4.3 carbon 5.2 Al2O3 2.2 Y2O3 B35 35.9 silicon carbide 65 silicon carbide 2000 582 174 — 36.2 silicon nitride 35 boron nitride 14.3 boron carbide 6.2 carbon 5.2 Al2O3 2.2 Y2O3 -
TABLE 1-2 Phase composition of Hot-pressing Bending Elastic Fracture Sample Composition of raw resulting material temperature strength modulus toughness No. material (wt %) (vol %) (° C.) (MPa) (GPa) (MPam½) B45 17.4 silicon carbide 55 silicon carbide 2000 471 127 — 48.6 silicon nitride 45 boron nitride 19.1 boron carbide 8.3 carbon 7 Al2O3 3 Al2O3 B55 60.2 silicon nitride 46.29 silicon carbide 2000 342 107 6 23.7 boron carbide 53.71 boron nitride 10.3 carbon 4 Al2O3 1.7 Y2O3 carbon 51.6 silicon carbide 75 silicon carbide 2000 420 217 5 25 42.6 boron nitride 25 boron nitride 4 Al2O3 1.7 Y2O3 carbon 74.8 silicon carbide 46.29 silicon carbide 2000 246 81 — 55 17.7 boron nitride 53.71 boron nitride 5.2 Al2O3 2.2 Y2O3 - B0, carbon 55 and carbon 25 are given in Table 1 as comparative examples. Among these, the hot-pressed sintered articles produced from silicon carbide-boron nitride powder mixtures displayed a three-point bending strength of approximately 250 MPa and a fracture toughness of 5 MPam ½, which were recognised as coming substantially below the values for all of the working examples.
- As has been described in the foregoing, the present invention relates to a silicon carbide-boron nitride composite material, which is obtained in accordance with an in-situ chemical reaction between silicon nitride, boron carbide and carbon, by moulding and sintering a powdered mixture containing each component, and a method for the manufacture of same. According to the present invention, the following exceptional merits can be obtained: 1) it is possible to manufacture and thereby to provide a silicon carbide-boron nitride composite material in which very fine boron nitride particles have been uniformly dispersed in a silicon carbide matrix; 2) using an uncomplicated process it is possible to obtain a silicon carbide-boron nitride composite material which exhibits high strength, a low elastic modulus, and high fracture toughness at room temperature, by utilising an in-situ chemical reaction between silicon nitride, boron carbide and carbon, mixing each component powder together and then hot-pressing the mixture; and 3) it is possible to manufacture a silicon carbide-boron nitride composite material of high performance, inexpensively.
Claims (4)
1. A silicon carbide-boron nitride composite material with fine boron nitride particles uniformly dispersed in a silicon carbide matrix, which synthesised according to an in-situ chemical reaction between silicon nitride, boron carbide and carbon,
said silicon carbide-boron nitride composite material is produced by molding a powder mixture containing the said components which are required in the in-situ chemical reaction, and sintering the molded mixture to obtain the sintered composite.
2. A silicon carbide-boron nitride composite material, which synthesised according to an in-situ chemical reaction between at least silicon nitride, boron carbide and carbon,
said silicon carbide-boron nitride composite material is produced by molding a powder comprising a silicon carbide, boron nitride or silicon nitride powder being added to a powder mixture containing the said components which are required in the in-situ chemical reaction between silicon nitride, boron carbide and carbon, and sintering the molded mixture to obtain the sintered composite comprising silicon carbide-boron nitride or silicon carbide-silicon nitride-boron nitride in which the phase composition is adjusted as required.
3. A silicon carbide-boron nitride composite material, which synthesised according to an in-situ chemical reaction between at least silicon nitride, boron carbide and carbon,
said silicon carbide-boron nitride composite material is produced by molding a powder comprising a silicon carbide or boron nitride powder being added to a powder mixture containing the said components which are required in an in-situ chemical reaction between silicon nitride, boron carbide and carbon, and sintering the molded mixture to obtain the sintered composite in which the phase composition is adjusted as required.
4. A method for manufacturing the composite material defined in any one of claims 1 through 3, which comprises mixing the components which are required in an in-situ chemical reaction between silicon nitride, boron carbide and carbon, adding further as required, at least one component selected from among silicon carbide, boron nitride or silicon nitride thereinto, molding the mixture, and sintering the molded mixture to manufacture a silicon carbide-boron nitride composite material or a silicon carbide-silicon nitride-boron nitride composite material.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6746748B2 (en) * | 2000-11-17 | 2004-06-08 | Ngk Insulators, Ltd. | Honeycomb structure and process for production thereof |
| US20090312173A1 (en) * | 2008-06-13 | 2009-12-17 | Saint-Gobain Ceramics & Plastics, Inc. | Volume-change resistant silicon oxy-nitride or silicon oxy-nitride and silicon nitride bonded silicon carbide refractory |
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| JP2006076858A (en) * | 2004-09-13 | 2006-03-23 | National Institute Of Advanced Industrial & Technology | Composite ceramics |
| US20060084566A1 (en) * | 2004-10-19 | 2006-04-20 | General Electric Company | Multiphase ceramic nanocomposites and method of making them |
| US7166550B2 (en) * | 2005-01-07 | 2007-01-23 | Xin Chen | Ceramic composite body of silicon carbide/boron nitride/carbon |
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| CN102821898B (en) * | 2010-10-27 | 2015-01-28 | 住友电工硬质合金株式会社 | Cubic boron nitride sintered body and cubic boron nitride (cbn) sintered body tool |
| US9446989B2 (en) | 2012-12-28 | 2016-09-20 | United Technologies Corporation | Carbon fiber-reinforced article and method therefor |
| CN104276823B (en) * | 2013-07-12 | 2016-03-23 | 中国科学院上海硅酸盐研究所 | High insulating silicon carbide/boron nitride ceramic material and preparation method thereof |
| JP5911837B2 (en) * | 2013-10-30 | 2016-04-27 | 富士フイルム株式会社 | Medical device repair information management apparatus, operation method and control program thereof, and repair information management system |
| US9732005B2 (en) | 2014-04-07 | 2017-08-15 | United Technologies Corporation | Method of forming in-situ boron nitride for ceramic matrix composite environmental protection |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| US4080415A (en) * | 1976-11-22 | 1978-03-21 | The Carborundum Company | Method of producing high density silicon carbide product |
| US4135938A (en) * | 1977-03-31 | 1979-01-23 | The Carborundum Company | High density thermal shock resistant sintered silicon carbide |
| US4701427A (en) * | 1985-10-17 | 1987-10-20 | Stemcor Corporation | Sintered silicon carbide ceramic body of high electrical resistivity |
| JPH03150267A (en) * | 1989-11-06 | 1991-06-26 | Eagle Ind Co Ltd | Silicon carbide sliding material |
| JP3150267B2 (en) | 1995-03-31 | 2001-03-26 | ティーディーケイ株式会社 | Optical recording medium |
| JP4312293B2 (en) * | 1999-03-16 | 2009-08-12 | 独立行政法人科学技術振興機構 | Silicon carbide ceramic composite material and manufacturing method thereof |
-
2000
- 2000-06-16 JP JP2000180931A patent/JP3607939B2/en not_active Expired - Lifetime
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US6746748B2 (en) * | 2000-11-17 | 2004-06-08 | Ngk Insulators, Ltd. | Honeycomb structure and process for production thereof |
| US20090312173A1 (en) * | 2008-06-13 | 2009-12-17 | Saint-Gobain Ceramics & Plastics, Inc. | Volume-change resistant silicon oxy-nitride or silicon oxy-nitride and silicon nitride bonded silicon carbide refractory |
| US8003557B2 (en) | 2008-06-13 | 2011-08-23 | Saint-Gobain Ceramics & Plastics, Inc. | Volume-change resistant silicon oxy-nitride or silicon oxy-nitride and silicon nitride bonded silicon carbide refractory |
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| US6764974B2 (en) | 2004-07-20 |
| JP2002003276A (en) | 2002-01-09 |
| US20030211930A1 (en) | 2003-11-13 |
| JP3607939B2 (en) | 2005-01-05 |
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