JPH02157163A - Production of composite silicon nitride combined sintered body - Google Patents
Production of composite silicon nitride combined sintered bodyInfo
- Publication number
- JPH02157163A JPH02157163A JP63311445A JP31144588A JPH02157163A JP H02157163 A JPH02157163 A JP H02157163A JP 63311445 A JP63311445 A JP 63311445A JP 31144588 A JP31144588 A JP 31144588A JP H02157163 A JPH02157163 A JP H02157163A
- Authority
- JP
- Japan
- Prior art keywords
- silicon nitride
- whiskers
- sintered body
- si3n4
- coil
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 229910052581 Si3N4 Inorganic materials 0.000 title claims abstract description 45
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 title claims description 40
- 239000002131 composite material Substances 0.000 title claims description 10
- 238000004519 manufacturing process Methods 0.000 title claims description 10
- 239000000843 powder Substances 0.000 claims abstract description 13
- 238000005245 sintering Methods 0.000 claims abstract description 13
- 238000000034 method Methods 0.000 claims description 13
- 239000002994 raw material Substances 0.000 claims description 3
- 238000005452 bending Methods 0.000 abstract description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 abstract description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 3
- 229910002804 graphite Inorganic materials 0.000 abstract description 2
- 239000010439 graphite Substances 0.000 abstract description 2
- 239000011261 inert gas Substances 0.000 abstract description 2
- 238000000465 moulding Methods 0.000 abstract description 2
- 230000035939 shock Effects 0.000 abstract description 2
- 239000008246 gaseous mixture Substances 0.000 abstract 1
- 229910052757 nitrogen Inorganic materials 0.000 abstract 1
- 239000007858 starting material Substances 0.000 abstract 1
- 239000011159 matrix material Substances 0.000 description 10
- 239000000463 material Substances 0.000 description 5
- 230000000694 effects Effects 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 3
- 238000007796 conventional method Methods 0.000 description 3
- 239000013078 crystal Substances 0.000 description 3
- 238000013001 point bending Methods 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 238000007731 hot pressing Methods 0.000 description 2
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 2
- 229910010271 silicon carbide Inorganic materials 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- 241000721701 Lynx Species 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 125000004435 hydrogen atom Chemical class [H]* 0.000 description 1
- 230000002706 hydrostatic effect Effects 0.000 description 1
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 1
- 239000011812 mixed powder Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000011863 silicon-based powder Substances 0.000 description 1
- 238000007655 standard test method Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
Abstract
Description
【発明の詳細な説明】
（産業上の利用分野）
本発明は、機械的強度に優れた窒化珪素複合焼結体に関
する。DETAILED DESCRIPTION OF THE INVENTION (Field of Industrial Application) The present invention relates to a silicon nitride composite sintered body having excellent mechanical strength.
（従来の技術）
窒化珪素（ＳｉＪ４）は、耐熱性、耐熱衝撃性、耐蝕性
に優れているため、高温構造材料として期待されている
材料である。(Prior Art) Silicon nitride (SiJ4) is a material expected to be used as a high-temperature structural material because it has excellent heat resistance, thermal shock resistance, and corrosion resistance.
しかしながら、窒化珪素焼結体を製造する場合、窒化珪
素粉末のみで高密度、高強度を達成するのは困難である
ため、従来より酸化マグネシウムなどの焼結助剤を添加
する方法、ホットプレスを行う方法等が試みられている
が、いずれにおいても充分な強度向上効果が得られてい
ない。さらに強度の向上を図ることを目的として、マト
リックスとしての窒化珪素粉末に炭化珪素等の単結晶繊
維（ウィスカー）を添加して焼結し、複合焼結体とする
ことが試みられている。該方法は、上記従来の焼結助剤
を用いる方法、ホットプレスを行う方法等に比べると、
より優れた機械的強度を達成することができる。However, when manufacturing silicon nitride sintered bodies, it is difficult to achieve high density and high strength using only silicon nitride powder, so conventional methods include adding sintering aids such as magnesium oxide, and hot pressing. Several methods have been tried, but none of them have been able to achieve a sufficient strength-improving effect. In order to further improve the strength, attempts have been made to add single crystal fibers (whiskers) of silicon carbide or the like to silicon nitride powder as a matrix and sinter it to produce a composite sintered body. This method has the following advantages compared to the conventional method using a sintering aid, hot pressing method, etc.
Better mechanical strength can be achieved.
さらに、特開昭５６−９２１８０号には、針状の窒化珪
素ウィスカーを窒化珪素粉末に添加して混合し、得られ
た原料粉末を成形して焼結することからなる焼結体の製
造方法が提案されている。Furthermore, JP-A No. 56-92180 discloses a method for manufacturing a sintered body, which comprises adding and mixing acicular silicon nitride whiskers to silicon nitride powder, shaping and sintering the obtained raw material powder. is proposed.
該方法においては、マトリックスと同材料のウィスカー
を用いるため、炭化珪素等のウィスカーを使用する場合
に比べて、ウィスカーとマトリックスとの接着性が優れ
ており、機械的強度もさらに向上している。In this method, since whiskers made of the same material as the matrix are used, the adhesion between the whiskers and the matrix is superior to that in the case of using whiskers such as silicon carbide, and the mechanical strength is further improved.
（発明が解決しようとする課題）
しかしながら、上記の特開昭５６−９２１８０号の方法
においても、充分な機械的強度は達成されておらず、特
に、曲げ強度及び破壊靭性に関してはさらに向上させる
ことが望まれている。そして、これは同材料のウィスカ
ーを用いた場合でも、ウィスカーとマトリックスとの接
着性に関して未だ充分ではないためであると考えられて
いる。ウィスカーとマトリックスとの接着性を改善する
ために、ウィスカーの表面にカーボン等のコーティング
を施す試みが為されているが、これらの方法においても
、ウィスカーと７トリツクスとの接着性の改善効果は充
分とは言えない。(Problems to be Solved by the Invention) However, even with the method of JP-A-56-92180, sufficient mechanical strength has not been achieved, and in particular, it is necessary to further improve the bending strength and fracture toughness. is desired. This is thought to be because even when whiskers made of the same material are used, the adhesion between the whiskers and the matrix is still insufficient. In order to improve the adhesion between the whiskers and the matrix, attempts have been made to coat the whisker surface with carbon or other materials, but these methods have not been able to sufficiently improve the adhesion between the whiskers and the 7trix. It can not be said.
従って、本発明は、窒化珪素ウィスカーを添加して焼結
してなる窒化珪素複合焼結体の製造において、ウィスカ
ーとマトリックスの接着性をさらに改善し、機械的強度
、特に曲げ強度及び破壊靭性に優れた窒化珪素複合焼結
体を製造することを目的とする。Therefore, the present invention further improves the adhesion between the whiskers and the matrix in the production of a silicon nitride composite sintered body made by adding and sintering silicon nitride whiskers, and improves mechanical strength, especially bending strength and fracture toughness. The purpose is to manufacture an excellent silicon nitride composite sintered body.
（課題を解決するための手段）
上記の目的を達成するために、本発明の窒化珪素複合焼
結体の製造方法は、３〜５０容量％のコイル状の窒化珪
素ウィスカーを含み、残部が窒化珪素粉末である原料粉
末を成形し、焼結することを特徴とする。(Means for Solving the Problems) In order to achieve the above object, the method for manufacturing a silicon nitride composite sintered body of the present invention includes 3 to 50% by volume of coiled silicon nitride whiskers, and the remainder is nitrided. It is characterized by molding and sintering raw material powder, which is silicon powder.
コイル状の窒化珪素ウィスカーは、例えば、黒鉛の薄板
上に、約１２００°Ｃの温度でアンモニア、水素、塩素
、気化珪素よりなる混合気体を流すことにより形成する
ことができる。特に、太さが１〜５μｍ、コイルの径が
１０〜５０μｍ、長さが５０μｍ〜１００ μｍである
窒化ケイ素ウィスカーを使用すると、ウィスカーとマＩ
・リンクスとの接着性がより良好となり、より高い強度
が達成されるため好ましい。Coiled silicon nitride whiskers can be formed, for example, by flowing a gas mixture of ammonia, hydrogen, chlorine, and vaporized silicon over a thin graphite plate at a temperature of about 1200°C. In particular, when using silicon nitride whiskers with a thickness of 1 to 5 μm, a coil diameter of 10 to 50 μm, and a length of 50 μm to 100 μm, the whisker and the
- It is preferable because it has better adhesion with Lynx and achieves higher strength.
窒化珪素ウィスカーの添加量は、３容量％未満では充分
な強度向上効果が得られず、５０容量％を超えてもそれ
以上効果が上がらず、却って曲げ強度及び破壊靭性が低
下するため、３〜５０容量％とする。If the amount of silicon nitride whiskers added is less than 3% by volume, sufficient strength improvement effect will not be obtained, and if it exceeds 50% by volume, the effect will not increase any further, and the bending strength and fracture toughness will decrease, so It is assumed to be 50% by volume.
マトリックスとしては、α相を９０重量％以上含む窒化
珪素粉末を使用するのが好ましい。これは、窒化珪素の
焼結には窒化珪素のα相よりβ相への転移が関与するた
めである。As the matrix, it is preferable to use silicon nitride powder containing 90% by weight or more of α phase. This is because sintering of silicon nitride involves transition from the α phase to the β phase of silicon nitride.
焼結は、窒化珪素の分解、酸化等を防止するために、窒
素ガスまたは不活性ガス雰囲気下のような、非酸化性雰
囲気下で行うのが好ましい。Sintering is preferably performed in a non-oxidizing atmosphere, such as a nitrogen gas or inert gas atmosphere, in order to prevent decomposition, oxidation, etc. of silicon nitride.
焼結温度は、１７００°Ｃ未満では高密度の焼結体が得
られにくく、１８５０’Ｃより高くなると、窒化珪素が
分解する虞れがあるため、１７００〜１８５０’Ｃで行
うのが好ましい。If the sintering temperature is lower than 1700°C, it will be difficult to obtain a high-density sintered body, and if it is higher than 1850°C, silicon nitride may decompose.
（作用）
本発明の窒化珪素複合焼結体の製造方法においては、マ
トリックスとしての窒化珪素粉末に添加する窒化珪素ウ
ィスカーがコイル状であるため、ウィスカーとマトリッ
クスとの接着性が良好であり、機械的強度、特に曲げ強
度及び破壊靭性が高い。(Function) In the method for manufacturing a silicon nitride composite sintered body of the present invention, since the silicon nitride whiskers added to the silicon nitride powder as a matrix are coiled, the adhesion between the whiskers and the matrix is good, and the mechanical High mechanical strength, especially bending strength and fracture toughness.
（実施例） 以下、本発明を実施例によりさらに詳細に説明する。(Example) Hereinafter, the present invention will be explained in more detail with reference to Examples.
実施例：
第１図及び第２図の拡大図に１として示すような形状を
有する太さ約１μｍで、コイルの径が約１０μｍのコイ
ル状窒化珪素ウィスカー１０容量％と、α相を９０重量
％含む窒化珪素粉末９０容量％を秤取して、均一になる
まで混合する。この混合粉末を、ラバープレス装置を用
いて、３ｔ／ｃ＋ｆｌの静水圧で所定の形状に成形した
後、常法にしたがってＮ２ガス雰囲気中、１８００°Ｃ
で４時間焼結を行って目的とする焼結体を得る。Example: 10% by volume of coiled silicon nitride whiskers having a shape as shown as 1 in the enlarged views of FIGS. 1 and 2, having a thickness of about 1 μm and a coil diameter of about 10 μm, and 90% by weight of α phase. % silicon nitride powder containing 90% by volume is weighed out and mixed until uniform. This mixed powder was molded into a predetermined shape using a rubber press machine under a hydrostatic pressure of 3t/c+fl, and then heated to 1800°C in a N2 gas atmosphere according to a conventional method.
Sintering is performed for 4 hours to obtain the desired sintered body.
上記により製造された焼結体（本発明品）及びコイル状
窒化珪素ウィスカーの代わりに針状の窒化珪素ウィスカ
ーを使用すること以外は上記実施例と同様の方法により
製造した焼結体（比較品）の３点曲げ強度をＪＩＳ規格
の試験法により評価したところ、本発明品の焼結体は、
比較品の焼結体に比べて優れた３点曲げ強度を示した。The sintered body manufactured as described above (product of the present invention) and the sintered body manufactured by the same method as in the above example except that needle-shaped silicon nitride whiskers were used instead of the coiled silicon nitride whiskers (comparative product). ) The three-point bending strength of the sintered body of the present invention was evaluated using the JIS standard test method.
It exhibited superior three-point bending strength compared to the comparative sintered body.
また、上記の本発明品の焼結体及び比較品の焼結体のに
＋ｃ（臨界応力拡大係数）を測定したところ、本発明品
の焼結体のＫＩＣは比較品に比べて高く、これは、本発
明品の焼結体の方が破壊靭性に優れていることを示す。In addition, when +c (critical stress intensity factor) was measured for the above-mentioned sintered body of the present invention product and comparative product, the KIC of the sintered body of the present invention product was higher than that of the comparison product. indicates that the sintered body of the present invention has better fracture toughness.
これらの結果より、コイル状のウィスカーを用いて製造
した焼結体の方が、針状のウィスカーを用いて製造した
焼結体よりも強度が高いことが明らかであり、コイル状
のウィスカーの方が針状結晶のウィスカーよりもマトリ
ックスに対する接着性に優れていることが類推される。From these results, it is clear that the sintered body manufactured using coiled whiskers has higher strength than the sintered body manufactured using needle-shaped whiskers. It can be inferred that the adhesion to the matrix is superior to that of needle-like crystal whiskers.
試験例：
上記実施例の方法により、コイル状の窒化珪素ウィスカ
ーの添加量及び焼結温度を、下記の第１表に示すように
変化させて焼結体を製造し、各々の焼結体の３点曲げ強
度及びＫＩＣを調べた。Test example: Sintered bodies were manufactured by the method of the above example, changing the amount of coiled silicon nitride whiskers added and the sintering temperature as shown in Table 1 below. Three-point bending strength and KIC were investigated.
結果を下記の第１表に示す。The results are shown in Table 1 below.
第１表
上記の第１表より、窒化珪素ウィスカーの添加量は、２
容量％以下では、破壊靭性が著しく低下し、６０容量％
以上では曲げ強度及び破壊靭性の両方が著しく低下する
ため、３〜５０容量％が適当であることが明らかである
。Table 1 From Table 1 above, the amount of silicon nitride whiskers added is 2
Below 60% by volume, the fracture toughness decreases significantly.
It is clear that 3 to 50% by volume is appropriate since both the bending strength and fracture toughness are significantly reduced above.
（発明の効果）
本発明の窒化珪素複合焼結体の製造方法は、コイル状の
窒化珪素ウィスカーが添加された窒化珪素粉末を焼結す
ることがらなり、得られた焼結体の強度、特に曲げ強度
及び破壊靭性が著しく向上するため、窒化珪素焼結体の
利用分野がさらに拡大し、耐熱性、耐熱衝撃性、耐蝕性
に優れるという窒化珪素焼結体の性質を有し、しかも機
械的強度が著しく向上された焼結晶の製造が可能となる
。(Effects of the Invention) The method for producing a silicon nitride composite sintered body of the present invention involves sintering silicon nitride powder to which coiled silicon nitride whiskers are added, and the strength of the obtained sintered body, especially As the bending strength and fracture toughness are significantly improved, the field of application of silicon nitride sintered bodies will further expand. It becomes possible to produce sintered crystals with significantly improved strength.
第１図及び第２図は、本発明の一実施例の窒化珪素複合
焼結体の製造方法に使用される、コイル状窒化珪素ウィ
スカーを示す拡大図である。
１・・・コイル状窒化珪素ウィスヵ一FIGS. 1 and 2 are enlarged views showing coiled silicon nitride whiskers used in a method for manufacturing a silicon nitride composite sintered body according to an embodiment of the present invention. 1... Coiled silicon nitride whisker
Claims (1)
、残部が窒化珪素粉末である原料粉末を成形し、焼結す
ることを特徴とする窒化珪素複合焼結体の製造方法。A method for manufacturing a silicon nitride composite sintered body, comprising forming and sintering a raw material powder containing 3 to 50% by volume of coiled silicon nitride whiskers, the remainder being silicon nitride powder.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63311445A JPH0818877B2 (en) | 1988-12-09 | 1988-12-09 | Method for manufacturing silicon nitride composite sintered body |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63311445A JPH0818877B2 (en) | 1988-12-09 | 1988-12-09 | Method for manufacturing silicon nitride composite sintered body |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH02157163A true JPH02157163A (en) | 1990-06-15 |
| JPH0818877B2 JPH0818877B2 (en) | 1996-02-28 |
Family
ID=18017301
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP63311445A Expired - Lifetime JPH0818877B2 (en) | 1988-12-09 | 1988-12-09 | Method for manufacturing silicon nitride composite sintered body |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0818877B2 (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH05279138A (en) * | 1992-03-31 | 1993-10-26 | Kyocera Corp | Fiber-reinforced ceramics and their production |
-
1988
- 1988-12-09 JP JP63311445A patent/JPH0818877B2/en not_active Expired - Lifetime
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH05279138A (en) * | 1992-03-31 | 1993-10-26 | Kyocera Corp | Fiber-reinforced ceramics and their production |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0818877B2 (en) | 1996-02-28 |
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