JPS6121964A - Alumina sintered body and manufacture - Google Patents
Alumina sintered body and manufactureInfo
- Publication number
- JPS6121964A JPS6121964A JP59144795A JP14479584A JPS6121964A JP S6121964 A JPS6121964 A JP S6121964A JP 59144795 A JP59144795 A JP 59144795A JP 14479584 A JP14479584 A JP 14479584A JP S6121964 A JPS6121964 A JP S6121964A
- Authority
- JP
- Japan
- Prior art keywords
- alumina
- sintered body
- silicon carbide
- particle size
- average particle
- 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.)
- Pending
Links
Abstract
(57)【要約】本公報は電子出願前の出願データであるた
め要約のデータは記録されません。(57) [Summary] This bulletin contains application data before electronic filing, so abstract data is not recorded.
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は、主成分が炭化ケイ素とアルミナ微粉の均質な
組成か−ろ成るアルミナ質焼結体およびその製造方法で
あって、特に破かいしん性が優れており半導体パッケー
ジ、耐熱性ＩＣ基板および各種の機械部品などに好適の
アルミナ質焼結体およびその製造方法に関する。Detailed Description of the Invention [Industrial Field of Application] The present invention relates to an alumina sintered body whose main components are silicon carbide and alumina fine powder with a homogeneous composition, and a method for producing the same. The present invention relates to an alumina sintered body that has excellent properties and is suitable for semiconductor packages, heat-resistant IC boards, various mechanical parts, etc., and a method for manufacturing the same.
アルミナ質結体は、一般に常温強度、耐熱性、硬度、化
学的安定性及び電気的絶縁性に優れた材料であり、耐蝕
耐摩耗部品、電子工業用部品、点火栓用部品などに広く
使用されている。なかでもアルミナ焼結体は、高温部品
として注目されているが、高温下における強度、硬度、
クリ−１特性、破かいしん性、さらに耐熱衝撃性が十分
でなく、また電子工業用部品としては高速・高密度化に
より熱伝導率（λ）が高い基板が要求されているにも拘
らずλは低く放熱性が劣っている。Alumina aggregates are generally materials with excellent room-temperature strength, heat resistance, hardness, chemical stability, and electrical insulation, and are widely used in corrosion-resistant and wear-resistant parts, electronic industry parts, spark plug parts, etc. ing. Among these, alumina sintered bodies are attracting attention as high-temperature parts, but their strength, hardness, and
Cree-1 characteristics, fracture resistance, and thermal shock resistance are insufficient, and even though substrates with high thermal conductivity (λ) are required for electronic industrial parts due to high speed and high density, λ is low and has poor heat dissipation.
そこで上記問題点を解決すべく高純度のアルミナ粉末を
高温高圧下で焼結するホットプレス法によるアルミナ焼
結体、アルミナ単結晶製品などが検討されている。Therefore, in order to solve the above-mentioned problems, alumina sintered bodies and alumina single crystal products produced by a hot press method in which high-purity alumina powder is sintered under high temperature and pressure are being considered.
しかしながら、前記ホットプレス法くよる高純度アルミ
ナ焼結体は熱伝導性は向上するものの高温強度、破かい
しん性が今−歩十分でなく割れ易い。また前記単結晶製
品は熱伝導率、高温強度は改善されるがコストが極めて
高くなる。However, although the high-purity alumina sintered body produced by the hot pressing method has improved thermal conductivity, its high-temperature strength and fracture resistance are insufficient and it is easily broken. Further, although the single crystal product has improved thermal conductivity and high temperature strength, it is extremely expensive.
他方、アルミナにジルコニアを添加した複合焼結体又は
アルミナにウィスカーを混入した複合焼結体が提案され
ているが、前者の焼結体は放射性元素が共存し易いので
電子部品としての用途には適さず、後者の焼結体はライ
・νｆ入による方向性があり物性面で不利でありコスト
も高くなる。On the other hand, composite sintered bodies in which zirconia is added to alumina or composite sintered bodies in which whiskers are mixed in alumina have been proposed, but the former sintered bodies tend to contain radioactive elements, so they are not suitable for use as electronic components. The latter sintered body is unsuitable, and the latter sintered body has directionality due to lie/vf inclusion, which is disadvantageous in terms of physical properties and increases cost.
このようなことを考慮して水出願人は、先く「炭化珪素
が重量比て０，６〜４０％含有され、残部がアルミナを
主成分とする混合組成分で構成された炭化珪素含有のア
ルミナ質焼結体」に係る先行発明を提案している、そし
て上記炭化珪素含有のアルミナ質焼結体は主として常圧
焼結によりＳｉＣ粒子をＡＩｔｏ３中に均一に含有させ
て強度、硬度、熱伝導率及び＃熱衝撃性などを向上させ
ることを目的とする発明である。Taking these things into consideration, the applicant previously proposed that ``a silicon carbide-containing material containing 0.6 to 40% by weight of silicon carbide and a mixed composition with the remainder being alumina as a main component. The above-mentioned silicon carbide-containing alumina sintered body is produced by uniformly containing SiC particles in AIto3 mainly by pressureless sintering to improve strength, hardness, and heat resistance. This invention aims to improve conductivity, #thermal shock resistance, etc.
本発明は、前記従来技術の欠点を除去・改善し、さらに
先行発明により得られる炭化珪素含有のアルミナ質焼結
体の物性、殊に破かいしん性（ＫＩＣ）を一段と向上さ
せることを主目的として、半導体パッケージ、ＩＣ基板
及び機械部品などに好適のアルミナ質焼結体を前記特許
請求の範囲に記載の発明によって提案しようとするもの
である。The main purpose of the present invention is to eliminate and improve the drawbacks of the prior art, and further improve the physical properties, especially the fracture resistance (KIC), of the silicon carbide-containing alumina sintered body obtained by the prior invention. The present invention attempts to propose an alumina sintered body suitable for semiconductor packages, IC boards, mechanical parts, etc., by the invention described in the claims.
次に、本発明のアルミナ質焼結体について具体的に説明
する。Next, the alumina sintered body of the present invention will be specifically explained.
〔問題点を解決すべき手段およびその作用〕本発明によ
れば炭化ケイ素が重量比で０．６〜４０％含有されてお
り、残部がアルミナを主成分とする混合組成物で構成さ
れた炭化ケイ素含有のアルミナ質焼結体において、アル
ミナの粒径が１０／Ｊｍ以下である均質な組成であり、
破かいしん性（ＫＩＣ）が特に優れていることを特徴と
するアルミナ質焼結体を提供することができる。[Means for solving the problems and their effects] According to the present invention, a carbonized carbonaceous material containing silicon carbide in a weight ratio of 0.6 to 40% and the balance being a mixed composition mainly composed of alumina. The silicon-containing alumina sintered body has a homogeneous composition in which the alumina particle size is 10/Jm or less,
It is possible to provide an alumina sintered body characterized by particularly excellent fracture resistance (KIC).
すなわち、まず本発明によれば、アルミナ質常圧焼結体
に含まれる炭化珪素は重量比で０．５〜４０％の範囲で
あることが必要である。炭化珪素が０．５％より少ない
と炭化珪素を含んだことに基づく硬度、強度、破壊しん
性及び熱伝導率の改善が十分でなく、４０％より多いと
アルミナと炭化珪素の焼結性が困難となり高密度のアル
ミナ質常圧焼結体が得られにくく、仮に、高密度の焼結
体が得られても炭化珪素粒子とアルミナ粒子の粒子間に
おける不均一部分が極めて多くなり機械的性質と熱的性
質を大幅に低下せしめるからであり、なかでも、炭化珪
素が０．５〜２０％の範囲であるととが最吃好適な結果
が得られる。That is, first, according to the present invention, silicon carbide contained in the alumina pressureless sintered body needs to be in the range of 0.5 to 40% by weight. If the silicon carbide content is less than 0.5%, improvements in hardness, strength, fracture resistance, and thermal conductivity due to the inclusion of silicon carbide will not be sufficient, and if it is more than 40%, the sinterability of alumina and silicon carbide will be reduced. This makes it difficult to obtain a high-density alumina pressureless sintered body, and even if a high-density sintered body is obtained, there will be extremely large amounts of unevenness between the silicon carbide particles and the alumina particles, resulting in poor mechanical properties. This is because silicon carbide significantly reduces the thermal properties, and among these, the most preferable result is obtained when the silicon carbide content is in the range of 0.5 to 20%.
次に１本発明によれば残部、実質的にアルミナの粒径が
１０μｆｆｌ −０，，１μｍである均質な組成であっ
て、前記炭化ケイ素以外の主成分をなすものであること
が必要である。アルミナの平均粒径が１０μｍＪ″シ大
きいと粒界破かい面積が小さくなり、表面エネルギー（
ｒ＋ ）が小さくなる。Next, according to the present invention, the remainder must have a homogeneous composition in which the particle size of alumina is substantially 10 μffl −0, 1 μm, and must be a main component other than the silicon carbide. . When the average grain size of alumina is 10 μmJ'' larger, the grain boundary fracture area becomes smaller and the surface energy (
r+) becomes smaller.
一方、アルミナの平均粒径が１０μｍより小さいと、ア
ルミナとアルミナとの粒界面の接触面積が大きくなるた
め、表面エネルギー（ｒｉ）は大きくなる。それゆえ、
本発明のアルミナ質焼結体の破がいしん性が向上するも
°のと考えられる。それは表面エネルギー、すなわち塑
性変形による吸収エネルギー及び破かいの際放出される
エネルギー或いは相変態に伴うエネルギーなどとＫＩＣ
とは比例関係にあるからである。したがって本発明のア
ルミナ質焼結体のように破かいしん性の優れた焼結体を
得るには、アルミナの粒径をできるだけ小さくしかも均
一に分布させ粒間の気孔率を小さくすると共に、原則と
して結晶の選択配向をなくすることがＫｔｃを向上させ
ることになる。On the other hand, if the average particle size of alumina is smaller than 10 μm, the contact area of grain boundaries between alumina and alumina becomes large, and thus the surface energy (ri) becomes large. therefore,
It is believed that the fracture resistance of the alumina sintered body of the present invention is improved. It is surface energy, that is, absorbed energy due to plastic deformation, energy released during fracture, or energy associated with phase transformation, and KIC.
This is because they are in a proportional relationship. Therefore, in order to obtain a sintered body with excellent fracture resistance, such as the alumina sintered body of the present invention, the particle size of alumina must be made as small as possible and uniformly distributed to reduce the porosity between the grains. Eliminating preferential orientation of crystals improves Ktc.
つまり、アルミナとアルミナ又はアルミナと炭化ケイ素
の粒界に不連続層が形成されると粒界の破かいが起り易
くなることも考えられる。In other words, if a discontinuous layer is formed at the grain boundaries between alumina and alumina or between alumina and silicon carbide, cracking of the grain boundaries may be likely to occur.
一方１．アルミナの粒径が０，１μｍより小さいと十分
に密度が高いアルミナ質焼結体が得られにくい。On the other hand 1. If the particle size of alumina is smaller than 0.1 μm, it is difficult to obtain an alumina sintered body with a sufficiently high density.
なお、本発明によれば前記アルミナ粉体の結晶構造はα
型アルミナであることが望ましい。その理由は、α型ア
ルミナは高温における安定性が優れているからである。According to the present invention, the crystal structure of the alumina powder is α
Type alumina is preferred. The reason is that α-type alumina has excellent stability at high temperatures.
また、本発明によれば炭化ケイ素は主としてβ型結晶構
造をしているものであることが必要である。その理由は
β潤度化珪素は結晶系が立方晶系であることから粒子の
物理的性質忙おいて異方性を示さないことから安定した
ミクロ構造を有するアルミナ質焼結体が得られるからで
ある。また、アルミナの結晶構造はα型アルミナである
ことが好ましい。その理由はα型アルミナは高温におけ
る安定性が優れているからである。Furthermore, according to the present invention, silicon carbide must primarily have a β-type crystal structure. The reason for this is that β-hydrated silicon has a cubic crystal system and does not show anisotropy due to the physical properties of the particles, so an alumina sintered body with a stable microstructure can be obtained. It is. Further, the crystal structure of alumina is preferably α-type alumina. The reason is that α-type alumina has excellent stability at high temperatures.
本発明によれば、前記炭化ケイ素の平均粒径は０．１〜
２．０μｍであることが望ましい。According to the present invention, the average particle size of the silicon carbide is from 0.1 to
The thickness is preferably 2.0 μm.
また、炭化ケイ素の粒径が０．１μｍより小さいと凝集
性が極めて強くなり原料混合時における分散性が低くな
る。一方、膨化ケイ素の粒径が２．０μｍより大きいと
炭化ケイ素粒子とアルミナ粒子との粒子間における不均
一な部分が大きくなり、いわゆるミスマツチが起こり焼
結体の機械的及び熱的性質が劣化することになる。Furthermore, if the particle size of silicon carbide is smaller than 0.1 μm, the cohesiveness becomes extremely strong and the dispersibility during mixing of raw materials becomes low. On the other hand, if the particle size of the expanded silicon is larger than 2.0 μm, the non-uniformity between the silicon carbide particles and the alumina particles becomes large, resulting in so-called mismatch, which deteriorates the mechanical and thermal properties of the sintered body. It turns out.
また本発明によれば、前記炭化ケイ素の含有量は特に０
．５〜５．０重量％であることが好ましい。Further, according to the present invention, the content of silicon carbide is particularly 0.
．． It is preferably 5 to 5.0% by weight.
０．５重量％以下であると、アルミナの粒成長の制御が
しにくくなるため、粒界破かいが起こりにくい。When the amount is 0.5% by weight or less, it becomes difficult to control grain growth of alumina, so grain boundary fracture is less likely to occur.
一方、炭化ケイ素の含有量が５．０重量％以上であると
不連続層が増大し破かいしん性が低下することになる。On the other hand, if the content of silicon carbide is 5.0% by weight or more, the number of discontinuous layers increases and the fracture resistance decreases.
また、本発明によれば、炭化珪素はアルミナ質焼結体に
均一に分散されていることが好ましい。Further, according to the present invention, silicon carbide is preferably uniformly dispersed in the alumina sintered body.
その理由は、炭化珪素が均一に分散していないと、アル
ミナ質焼結体の物性が不均一となり、さらに、均一性が
著しく悪いとアルミナ質焼結体に未焼結部分が生じ、ア
ルミナ質常圧焼結体の機械的性質及び熱的性質に著しい
劣化を示すからである。The reason for this is that if silicon carbide is not uniformly dispersed, the physical properties of the alumina sintered body will be non-uniform, and if the uniformity is extremely poor, unsintered areas will occur in the alumina sintered body, and the alumina This is because the mechanical properties and thermal properties of the pressureless sintered body show significant deterioration.
本発明によれば、炭化珪素を含むアルミナ質焼結体の嵩
密度は、理論密度の９５％、好ましくは９７％以上であ
ることが好ましい。その理由は、理論密度が９５％より
少ないと前記焼結体の内部に気孔部分が多く存在するこ
とになり、熱伝導率が低下するからである。According to the present invention, the bulk density of the alumina sintered body containing silicon carbide is preferably 95% or more of the theoretical density, preferably 97% or more. The reason for this is that if the theoretical density is less than 95%, there will be many pores inside the sintered body, resulting in a decrease in thermal conductivity.
以上のように１本発明によれば炭化ケイ素を重量比で０
．５〜４０％含有したアルミナ質焼結体くおいて、特に
α型アルミナの粒径を１０μｍ以下とし、β型炭化ケイ
素の粒径をＱ、 ｌ−２，０μｍの微粉を均質混合した
原料を使用することにより、炭化ケイ素は本質的に極め
て硬い材料であることから炭化ケイ素を含んだアルミナ
質焼結体の硬度は向上し、その炭化ケイ素が細かい粒子
として均一に分散していることからアルミナ質常圧焼結
体の強度も向上する。また、炭化ケイ素とアルミナは化
学的組成と結晶構造その他の諸性質が異なる為にミクロ
的な炭化ケイ素粒子とアルミナ質粒子の間においては組
成的及び構造的不均一部分が生じ、これに基づいて破壊
のクラックが伝播したときにその伝播エネルギーを消費
してクラックの進展を防止することから破壊しん性が向
上する。さらＫ、炭化ケイ累は熱伝導率に優れた材料で
あることから炭化ケイ素を均一に含んだアルミナ質焼結
体の熱伝導率が改蕾される。As described above, according to the present invention, the weight ratio of silicon carbide is 0.
．． In the alumina sintered body containing 5 to 40%, in particular, the particle size of α-type alumina is set to 10 μm or less, the particle size of β-type silicon carbide is Q, and a raw material is homogeneously mixed with fine powder of 1-2.0 μm. By using silicon carbide, the hardness of the alumina sintered body containing silicon carbide improves, since silicon carbide is essentially an extremely hard material, and because the silicon carbide is uniformly dispersed as fine particles, alumina The strength of the pressureless sintered body is also improved. In addition, because silicon carbide and alumina have different chemical compositions, crystal structures, and other properties, compositional and structural nonuniformities occur between microscopic silicon carbide particles and alumina particles. When a fracture crack propagates, the propagation energy is consumed to prevent the crack from progressing, which improves fracture resistance. Furthermore, since silicon carbide is a material with excellent thermal conductivity, the thermal conductivity of an alumina sintered body uniformly containing silicon carbide is improved.
次に本発明のアルミナ質焼結体の製造方法について説明
する。Next, a method for producing an alumina sintered body according to the present invention will be explained.
本発明によれば炭化ケイ素粉末０．５〜４０重量％と残
部が粒径１０μｍ以下のアルミナ粉末を主成分とする組
成物を均一に混合し、このようＫして得られる均一混合
の組成物を所望の形状にした後、該成形体を１３００〜
１９００℃の温度で常圧焼結することを必要とする。According to the present invention, a uniformly mixed composition obtained by uniformly mixing a composition whose main components are 0.5 to 40% by weight of silicon carbide powder and the remainder being alumina powder with a particle size of 10 μm or less, and performing K in this manner. After shaping into a desired shape, the molded body was heated to 1300~
It requires pressureless sintering at a temperature of 1900°C.
炭化ケイ素粉を０．６〜４０重量％混入する理由、並び
にア／ｌ／ミナ粉末の粒径を１０μｍ以下にする理由は
、炭化珪素粉体の平均粒径が０．０１μｍより小さいと
凝集性が極めて強く混合における分散性が低いからであ
り、２．０μｍより大きいと炭化珪素粒子とアルミナ質
粒子の粒子間における不均一部分が大きくなりアルミナ
質常圧焼結体の機械的性質及び熱的性質が劣化するから
である。The reason for mixing 0.6 to 40% by weight of silicon carbide powder and the reason for setting the particle size of A/L/Mina powder to 10 μm or less is that if the average particle size of silicon carbide powder is smaller than 0.01 μm, it tends to coagulate. This is because the dispersibility during mixing is extremely strong and the dispersibility during mixing is low.If the diameter is larger than 2.0 μm, the non-uniformity between the silicon carbide particles and the alumina particles becomes large, which deteriorates the mechanical properties and thermal properties of the alumina pressureless sintered body. This is because the properties deteriorate.
本発明によれば、炭化珪素はアルミナ質焼結体に均一に
分散されていることが好ましい。その理由は、炭化珪素
が均一に分散していないと、アルミナ質焼結体の物性が
不均一となり、さらに、均一性が著しく悪いとアルミナ
質焼結体に未焼結部分が生じ、アルミナ質常圧焼結体の
機械的性質及炭化珪素を含んだアルミナ質常圧焼結体が
得られる。According to the present invention, silicon carbide is preferably uniformly dispersed in the alumina sintered body. The reason for this is that if silicon carbide is not uniformly dispersed, the physical properties of the alumina sintered body will be non-uniform, and if the uniformity is extremely poor, unsintered areas will occur in the alumina sintered body, and the alumina Mechanical properties of a pressureless sintered body and an alumina pressureless sintered body containing silicon carbide are obtained.
このようにして得られる均一混合の組成物に水又はベン
ゼン、アセトン、アルコール、トリクロルエチレン、ト
ルエン、キンレンなどの有ｍ 溶剤と必要により分散剤
を添加し、ボールミル、アトライター、ホモミキサー、
振動ミμ、コロイドミル１ヘンシエルミキサー、高速ミ
キサーなどの１種又は２種以上の混合機を用いて均一に
混合することが重要である。さらに、混合の初期又は途
中の段階で成形助剤たとえばポリエチレングリコール、
ポリビニールアルコール、メチルセルローズ、グリセリ
ン、澱粉、アラビアゴム、フェノール樹脂、カーポワ、
ソクス、ステアリン酸、パラフィンエマルシコンなどを
添加すると成形性が向上する。To the homogeneously mixed composition thus obtained, water or a solvent such as benzene, acetone, alcohol, trichloroethylene, toluene, quintylene, etc., and a dispersant if necessary are added, and the mixture is processed using a ball mill, attritor, homomixer, etc.
It is important to mix uniformly using one or more types of mixers such as a vibrating Miμ, a Colloid Mill 1 Henschel mixer, or a high-speed mixer. Furthermore, forming aids such as polyethylene glycol may be added at the initial or intermediate stage of mixing.
Polyvinyl alcohol, methylcellulose, glycerin, starch, gum arabic, phenolic resin, Capois,
Addition of sox, stearic acid, paraffin emulsion, etc. improves moldability.
成形はたとえば、金型による加圧成形、ラバー成形、イ
ンジェクション成形、押出し成形、鋳込み成形、ドクタ
ーブレード法、カレンダー法、ベーパーディッピング法
などによって行なわれ、所望の成形体が得られる。Molding is carried out by, for example, pressure molding using a mold, rubber molding, injection molding, extrusion molding, casting molding, a doctor blade method, a calendar method, a vapor dipping method, etc. to obtain a desired molded product.
また本発明によれば、前記成形体は水素、加湿水素、窒
素、アルゴン、ヘリウムの１種又は２種以上のガスを含
む雰囲気で常圧焼成することができるが、加湿水素中が
最も好ましい。また、前記雰囲気中にＡＩ！ｏ、”５ｉ
Ｏ１ｃｏの１種又は２種以上のガスを含むことが好まし
い。その理由は、ＳｉＣ＋ＡｈＯｓ→３４０キＡ１ｚＯ
＋ＣＯの反応によりｓｔｃとＡｌ２Ｏ５が反応するが、
雰囲気中にＡｌ５ｏ、５ｉＯ１ＣＯなどのガス分圧が存
在するとＳｉＣとＡ１１０１の反応が抑制され緻密なＳ
ｉＣを含んだアルミナ質常圧焼結体が得られるからであ
る。また、前記成形体を重量比で炭化珪素０．５〜２８
．２％とアルミナ７１．８〜９９．５９６の混合物中に
埋め込んで焼成することが可能である。その理由は焼成
時に前記炭化珪素とアルミナとの混合物中で炭化珪素と
アルミナとの反応が生じ、ＡｈＯｌＳｉｎ、ＣＯのガス
が発生して前記成形体中におけるＳｉＣとＡｈＯｓとの
反応が抑制され緻密なＳＩＣが容易に、かつ安価に得ら
れるからである。Further, according to the present invention, the molded body can be fired at normal pressure in an atmosphere containing one or more gases of hydrogen, humidified hydrogen, nitrogen, argon, and helium, but humidified hydrogen is most preferred. Also, AI in the atmosphere! o,”5i
It is preferable that one or more types of O1co gases are included. The reason is that SiC + AhOs → 340K A1zO
stc and Al2O5 react due to +CO reaction,
When a partial pressure of a gas such as Al5o or 5iO1CO exists in the atmosphere, the reaction between SiC and A1101 is suppressed and the dense S
This is because an alumina pressureless sintered body containing iC can be obtained. In addition, the molded body has a weight ratio of silicon carbide of 0.5 to 28
．． It is possible to embed it in a mixture of 2% and 71.8-99.596 alumina and sinter it. The reason for this is that during firing, a reaction between silicon carbide and alumina occurs in the mixture of silicon carbide and alumina, gases of AhOlSin and CO are generated, and the reaction between SiC and AhOs in the compact is suppressed, resulting in a dense structure. This is because SIC can be obtained easily and at low cost.
そして本発明によれば、′補記成形体’ｉ １１１０〜
１９００℃の温度範囲において常圧焼結することが好ま
しい。その理由は１３００℃より低いとアルミナ粉体と
炭化珪素粉体の焼結性が低く十分に緻密な焼結体が得ら
れず、また、１９００°Ｃより高いと炭化珪素の粒子内
に不純物が拡散してアルミナ質常圧焼結体の熱伝導率が
大きく低下するからであり、最も好ましくは１４００〜
１６００″Ｃの温度範囲である。According to the present invention, 'supplementary molded body' i 1110~
Pressureless sintering is preferably performed in a temperature range of 1900°C. The reason for this is that if the temperature is lower than 1300°C, the sinterability of the alumina powder and silicon carbide powder is low and a sufficiently dense sintered body cannot be obtained. This is because the thermal conductivity of the alumina pressureless sintered body decreases greatly due to diffusion, and the most preferable range is 1400~
The temperature range is 1600″C.
本発明によれば前記炭化ケイ素粉体は主としてβ型結晶
構造をしており、その平均粒径が０．０１〜２．０μ′
ｍであって、残部が平均粒径０．０６〜１０μｍのα型
結晶構造のアルミナを主成分とする組成物を出発原料と
することが特に好ましい。According to the present invention, the silicon carbide powder mainly has a β-type crystal structure and has an average particle size of 0.01 to 2.0 μ'.
It is particularly preferable to use as a starting material a composition whose main component is alumina having an α-type crystal structure with an average particle diameter of 0.06 to 10 μm.
このようにして得られるアルミナ質焼結体はその嵩密度
が理論密度の９５％以上、特に好ましくは９８％以上で
あって、破かいじん性（Ｋｒｃ）が８−５ ＭＰａ １
１山以上であることを特徴とするものである。The alumina sintered body thus obtained has a bulk density of 95% or more, particularly preferably 98% or more of the theoretical density, and a fracture toughness (Krc) of 8-5 MPa 1
It is characterized by having one or more mountains.
次に本発明の実施例について説明する。Next, examples of the present invention will be described.
実施例１
平均粒径０．８μｍのβ型炭化珪素を重量比で０〜２０
％と平均粒径０．４μｍのα型アルミナを重量比で７８
〜９８％及び平均粒径２．０μｍの５１０２を重量比で
２％の配合物１に５種類用意し、各配合物１００ｇに対
し、水を１０ｏｆ添加し、ポリエチレングリコ−Ａ／Ｉ
Ｆとポリビニ−μアルコーＩＶｚｙ及びステアリン酸を
０．６ｇ添加してボールミμ中で２４時間聞易した。前
記混合物をスプレードフイヤにて乾燥造粒し、金型成形
法により１．５ ｔ／ｄの成形圧φ４０ Ｘ ５ ｔの
成形体を得た。前記成形体を管状炉に挿入し、加湿水素
気流中において１６００°Ｃの温度で１時間焼成してア
ルミナ質常圧焼結体を得た。Example 1 β-type silicon carbide with an average particle size of 0.8 μm in a weight ratio of 0 to 20
% and α-type alumina with an average particle size of 0.4 μm in weight ratio of 78
Five types of 5102 with a weight ratio of 2% and an average particle size of 2.0 μm were prepared in Formulation 1, and 10 of water was added to 100g of each formulation.
F, polyviny-μ alcohol IVzy and 0.6 g of stearic acid were added, and the mixture was incubated in a ball milli μ for 24 hours. The mixture was dried and granulated using a spray fire, and a molded body having a molding pressure of 1.5 t/d and a molding pressure of φ40×5 t was obtained by a molding method. The compact was inserted into a tubular furnace and fired in a humidified hydrogen stream at a temperature of 1600° C. for 1 hour to obtain an alumina atmospheric pressure sintered compact.
このようにして得られた焼結体の嵩密度、マイクロビッ
カース硬度計による硬度、インデンテーシ目ン法による
ＫＩｃ及びレーザフラッシュ法による熱伝導率を測定し
た結果を第１表に示した。また、得られた焼結体をＸ線
粉末回析したところ全ての実施例にβ型炭化珪素の含ま
れていることがみとめられた。Table 1 shows the results of measuring the bulk density of the sintered body thus obtained, the hardness by a micro Vickers hardness tester, the KIc by an indentation method, and the thermal conductivity by a laser flash method. Further, when the obtained sintered bodies were subjected to X-ray powder diffraction, it was found that β-type silicon carbide was contained in all the examples.
比較例１
平均粒径０．８μｍのβ型炭化珪素を重量比で５０％と
平均粒径０．４μｍのα型アルミナを重量比で４８％及
び平均粒径２．０μｍの５ｉ０２を重量比で２％の配合
物を用意し、実施例１と同様の方法で常圧焼結を行なっ
た結果を第１表に示した。Comparative Example 1 50% by weight of β-type silicon carbide with an average particle size of 0.8 μm, 48% by weight of α-type alumina with an average particle size of 0.4 μm, and 5i02 with an average particle size of 2.0 μm by weight. A 2% blend was prepared and pressureless sintered in the same manner as in Example 1. The results are shown in Table 1.
実施例２
平均粒径が０．８μｍの１５炭化珪素を重量比で５％と
平均粒径が０．４μｍのα型アルミナを重量比で９０％
又は９５％及び平均粒径的２．０μｍの５ｉＯｉ、Ｍｎ
Ｏ又はＭｇ、Ｏｆ、それぞれ重量比で５％の配合物を４
種類用意し、実施例１と同様の方法で混合し乾燥し成形
した後、加湿水素気流中で１５００℃の温度で２時間焼
成してアルミナ質常圧焼結体が得られた。このようにし
て得られた焼結体の物性を第２表に示す。Example 2 5% by weight of 15 silicon carbide with an average particle size of 0.8 μm and 90% by weight of α-type alumina with an average particle size of 0.4 μm
or 95% and 5iOi, Mn with an average particle size of 2.0 μm
O or Mg, Of, each 5% by weight formulation 4
Various types were prepared, mixed, dried and molded in the same manner as in Example 1, and then fired in a humidified hydrogen stream at a temperature of 1500° C. for 2 hours to obtain an alumina atmospheric pressure sintered body. Table 2 shows the physical properties of the sintered body thus obtained.
実施例８
炭化珪素の平均粒径と結晶構造、アルミナの平均粒径を
変化させてアルミナ質常圧焼結体を得た場合の結果を第
８表に示した。なお、炭化珪素、アルミナ及び５ｉＯｚ
の組成−重量比でそれぞれ２％、９６％及び２９６と一
定であり、配合物の配合、成形、焼成は実施例２と同様
に行なった。Example 8 Table 8 shows the results when an alumina pressureless sintered body was obtained by changing the average grain size and crystal structure of silicon carbide and the average grain size of alumina. In addition, silicon carbide, alumina and 5iOz
The composition-to-weight ratios were constant at 2%, 96%, and 296, respectively, and the compounding, molding, and baking were performed in the same manner as in Example 2.
比較例２
平均粒径が１０μｍのα型炭化珪素と平均粒径が０．４
μｍのα型アルミナを用いて焼結したアルミナ質常圧焼
結体の物性を第８表に示す。Comparative Example 2 α-type silicon carbide with an average particle size of 10 μm and an average particle size of 0.4
Table 8 shows the physical properties of an alumina pressureless sintered body sintered using μm α-type alumina.
実施例４
平均粒径が０．８μｍのβＦｊｊ１次化珪素を重量比で
８９６と平均粒径０．４μｍのα型アルミナを重量比で
９４９６及び平均粒径２．０μｍの５ｉ０２ｔ１″重量
比で８％の配合物を用意し、実施例１と同様の方法で混
合し成形した後、加湿水素気流中にて１５００″Ｃ又は
１６００℃で１時間焼成して得たアルミナ質常圧焼結体
の物性を第４表に示す。Example 4 βFjj primary silicon with an average particle size of 0.8 μm in a weight ratio of 896, α-type alumina with an average particle size of 0.4 μm in a weight ratio of 9496, and 5i02t1″ with an average particle size of 2.0 μm in a weight ratio of 8 % mixture was prepared, mixed and molded in the same manner as in Example 1, and then calcined in a humidified hydrogen stream at 1500''C or 1600℃ for 1 hour to obtain an alumina atmospheric pressure sintered body. The physical properties are shown in Table 4.
比較例８
実施例４と同一の成形体を加湿水素気流中にて１２６０
°Ｃ又は２０００°Ｃの温度で１時間焼成した結果を第
４表に示す。Comparative Example 8 The same molded body as in Example 4 was heated at 1260 °C in a humidified hydrogen stream.
Table 4 shows the results of firing for 1 hour at a temperature of 2000°C or 2000°C.
実施例５
平均粒径が０．８μｍのβ型炭化珪素を重量比で２％と
平均粒径が０．４μｍのα型アルミナを９６重量％と平
均粒径２μｍの５ｉ０２を重量比で２％の配合物を実施
例１と同様の方法で混合、成形した後、窒素、アルゴン
、加湿水素気流及びアルミナと炭化珪素混合物中に成形
体を埋めた場合について焼成した結果を第５表に示す。Example 5 2% by weight of β-type silicon carbide with an average particle size of 0.8 μm, 96% by weight of α-type alumina with an average particle size of 0.4 μm, and 2% by weight of 5i02 with an average particle size of 2 μm. Table 5 shows the results of mixing and molding the mixture in the same manner as in Example 1, and then sintering the molded body in a nitrogen, argon, humidified hydrogen stream, and a mixture of alumina and silicon carbide.
比較例４
実施例５と同一の方法で成形体を得た後、酸素気流中で
焼成した結果を第５表に示す。Comparative Example 4 A molded body was obtained in the same manner as in Example 5, and then fired in an oxygen stream. Table 5 shows the results.
第１表
（Ｉｔ） Ｋｘａ＝破壊しん性 （焼成温度１
６００℃ 加湿水素気流中）第２表
（焼成条件１５００℃ 加湿水素気流中）第８表
（焼成条件１６００℃ 加湿水素気流中）第４表
第５表
上記の実施例の結果から本明らかなように、従来のアル
ミナ質結体の破かいじん性は８．０ ＭＰａ ｆｉ”２
位であるのに対し、本発明のアルミナ焼結体の破かいし
ん性は８．８〜８．９ Ｍ Ｐ ａ ｍ 号と向上する
ことになる。Table 1 (It) Kxa = Fracture resistance (Sintering temperature 1
As is clear from the results of the above examples The fracture toughness of conventional alumina solids is 8.0 MPa fi”2
In contrast, the fracture resistance of the alumina sintered body of the present invention is improved to 8.8 to 8.9 MPam.
以上の結果からも明らかなように、本発明によれば、ア
ルミナ質焼結体中に炭化珪素を均一に分散させた常圧焼
結法により得られる焼結体は、特に機械的強度、熱伝導
性、電気絶縁性などが優れ、アルミナ質焼結体の優れた
電気的特性と炭化珪素質焼結体の優れた熱伝導性とが組
み合せられ、特に優れた破かいしん性と機械的強度を併
有するものである。As is clear from the above results, according to the present invention, the sintered body obtained by the pressureless sintering method in which silicon carbide is uniformly dispersed in the alumina sintered body has excellent mechanical strength and heat resistance. It has excellent conductivity and electrical insulation, and combines the excellent electrical properties of the alumina sintered body with the excellent thermal conductivity of the silicon carbide sintered body, resulting in particularly excellent fracture resistance and mechanical strength. It is held together.
Claims (1)
り、残部がアルミナを主成分とする混合組成物で構成さ
れた炭化ケイ素含有のアルミナ質焼結体において、アル
ミナの粒径が１０μｍ以下である均質な組成であって破
かいじん性（Ｋ＿Ｉ＿Ｃ）が特に優れていることを特徴
とするアルミナ質焼結体。 ２、嵩密度が理論密度の９５％以上、特に好ましくは９
７％であって、破かいじん性（Ｋ＿Ｉ＿Ｃ）が３．５Ｍ
Ｐａｍ＾１＾／＾２以上であることを特徴とする特許請
求の範囲第１項記載のアルミナ質焼結体。 ８、前記炭化ケイ素は主としてβ型結晶構造をしており
、その平均粒径は０．１〜２．０μｍであり、０．５〜
５％含有されるものであって、残部が平均粒径０．１〜
１０μｍのα型結晶構造のアルミナを主成分とする組成
物から構成されていることを特徴とする特許請求の範囲
第１項又は第２項記載のアルミナ質焼結体。 ４、炭化ケイ素粉末０．５〜４０重量％と残部が粒径１
０μｍ以下のアルミナ粉末を主成分とする組成物を均一
に混合し、このようにして得られる均一混合の組成物を
所望の形状に成形した後、該成形体を１３００〜１９０
０℃の温度で常圧焼結することを特徴とするアルミナ質
焼結体の製造方法。 ５、前記炭化ケイ素粉体は主としてβ型結晶構造をして
おり、その平均粒径が０．０１〜２．０μｍであり、０
．５〜５％含有されるものであって、残部が平均粒径０
．０５〜１０μｍのα型結晶構造のアルミナを主成分と
する組成物を出発原料とすることを特徴とする特許請求
の範囲第４項記載の製造方法。 ６、前記常圧焼結によって得られるアルミナ質焼結体は
その嵩密度が理論密度の９５％以上、特に好ましくは９
７％以上であって、破かいじん性（Ｋ＿Ｉ＿Ｃ）が３．
５ＭＰａｍ＾１＾／＾２以上であることを特徴とする特
許請求の範囲第４項又は第５項記載の製造方法。[Claims] 1. In a silicon carbide-containing alumina sintered body composed of a mixed composition containing 0.5 to 40% by weight of silicon carbide and the remainder being alumina as a main component. An alumina sintered body characterized by having a homogeneous composition in which the particle size of alumina is 10 μm or less and having particularly excellent fracture toughness (K_I_C). 2. Bulk density is 95% or more of the theoretical density, particularly preferably 9
7%, and the cracking toughness (K_I_C) is 3.5M.
The alumina sintered body according to claim 1, characterized in that Pam^1^/^2 or more. 8. The silicon carbide mainly has a β-type crystal structure, and its average particle size is 0.1 to 2.0 μm, and 0.5 to 2.0 μm.
It contains 5%, and the remainder has an average particle size of 0.1~
3. The alumina-based sintered body according to claim 1 or 2, characterized in that the alumina-based sintered body is composed of a composition whose main component is alumina having a 10 μm α-type crystal structure. 4. Silicon carbide powder 0.5 to 40% by weight and the remainder having a particle size of 1
After uniformly mixing a composition mainly composed of alumina powder of 0 μm or less and molding the uniformly mixed composition thus obtained into a desired shape, the molded body was heated to a temperature of 1300 to 190
A method for producing an alumina sintered body, characterized by sintering under normal pressure at a temperature of 0°C. 5. The silicon carbide powder mainly has a β-type crystal structure, and its average particle size is 0.01 to 2.0 μm.
．． It contains 5 to 5%, and the remainder has an average particle size of 0.
．． 5. The manufacturing method according to claim 4, wherein the starting material is a composition containing alumina having an α-type crystal structure of 05 to 10 μm as a main component. 6. The alumina sintered body obtained by the pressureless sintering has a bulk density of 95% or more of the theoretical density, particularly preferably 9.
7% or more, and the cracking toughness (K_I_C) is 3.
5. The manufacturing method according to claim 4 or 5, characterized in that it is 5 MPam^1^/^2 or more.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59144795A JPS6121964A (en) | 1984-07-11 | 1984-07-11 | Alumina sintered body and manufacture |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59144795A JPS6121964A (en) | 1984-07-11 | 1984-07-11 | Alumina sintered body and manufacture |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS6121964A true JPS6121964A (en) | 1986-01-30 |
Family
ID=15370628
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59144795A Pending JPS6121964A (en) | 1984-07-11 | 1984-07-11 | Alumina sintered body and manufacture |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS6121964A (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS6487552A (en) * | 1987-09-30 | 1989-03-31 | Koichi Niihara | Sic-al2o3 composite sintered body and its production thereof |
| US4889835A (en) * | 1987-09-30 | 1989-12-26 | Ngk Insulators, Ltd. | SiC-Al2 O3 composite sintered bodies and method of producing the same |
| JP2007111745A (en) * | 2005-10-20 | 2007-05-10 | Denso Corp | Method and device for discriminating and evaluating abnormality of welding workpiece |
| WO2017131159A1 (en) * | 2016-01-27 | 2017-08-03 | 住友大阪セメント株式会社 | Ceramic material and electrostatic chuck apparatus |
-
1984
- 1984-07-11 JP JP59144795A patent/JPS6121964A/en active Pending
Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS6487552A (en) * | 1987-09-30 | 1989-03-31 | Koichi Niihara | Sic-al2o3 composite sintered body and its production thereof |
| EP0311289A1 (en) * | 1987-09-30 | 1989-04-12 | Ngk Insulators, Ltd. | SiC-Al2O3 composite sintered bodies and method of producing the same |
| US4889834A (en) * | 1987-09-30 | 1989-12-26 | Ngk Insulators, Ltd. | SiC-Al2 O3 composite sintered bodies and method of producing the same |
| US4889835A (en) * | 1987-09-30 | 1989-12-26 | Ngk Insulators, Ltd. | SiC-Al2 O3 composite sintered bodies and method of producing the same |
| JP2507480B2 (en) * | 1987-09-30 | 1996-06-12 | 晧一 新原 | SiC-Al Lower 2 O Lower 3 Composite Sintered Body and Manufacturing Method Thereof |
| JP2007111745A (en) * | 2005-10-20 | 2007-05-10 | Denso Corp | Method and device for discriminating and evaluating abnormality of welding workpiece |
| WO2017131159A1 (en) * | 2016-01-27 | 2017-08-03 | 住友大阪セメント株式会社 | Ceramic material and electrostatic chuck apparatus |
| JP2017206436A (en) * | 2016-01-27 | 2017-11-24 | 住友大阪セメント株式会社 | Ceramic material, and electrostatic chuck device |
| JP6237954B1 (en) * | 2016-01-27 | 2017-11-29 | 住友大阪セメント株式会社 | Ceramic materials, electrostatic chuck device |
| US11387132B2 (en) | 2016-01-27 | 2022-07-12 | Sumitomo Osaka Cement Co., Ltd. | Ceramic material and electrostatic chuck device |
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