JPH0259473A - Production of aluminum nitride sintered body - Google Patents
Production of aluminum nitride sintered bodyInfo
- Publication number
- JPH0259473A JPH0259473A JP63207264A JP20726488A JPH0259473A JP H0259473 A JPH0259473 A JP H0259473A JP 63207264 A JP63207264 A JP 63207264A JP 20726488 A JP20726488 A JP 20726488A JP H0259473 A JPH0259473 A JP H0259473A
- Authority
- JP
- Japan
- Prior art keywords
- aluminum nitride
- sintering
- average particle
- sintered body
- particle size
- 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
- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 title claims abstract description 51
- 238000004519 manufacturing process Methods 0.000 title claims description 17
- 239000000843 powder Substances 0.000 claims abstract description 38
- 238000005245 sintering Methods 0.000 claims abstract description 34
- 239000002245 particle Substances 0.000 claims abstract description 24
- 239000012298 atmosphere Substances 0.000 claims abstract description 7
- 230000001590 oxidative effect Effects 0.000 claims description 3
- 238000000465 moulding Methods 0.000 abstract description 7
- 239000000203 mixture Substances 0.000 abstract description 5
- 238000000034 method Methods 0.000 description 22
- 239000002994 raw material Substances 0.000 description 10
- 238000002156 mixing Methods 0.000 description 8
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 5
- 239000012535 impurity Substances 0.000 description 5
- 239000001301 oxygen Substances 0.000 description 5
- 229910052760 oxygen Inorganic materials 0.000 description 5
- 239000000758 substrate Substances 0.000 description 5
- 238000010304 firing Methods 0.000 description 4
- 229910052751 metal Inorganic materials 0.000 description 4
- 239000002184 metal Substances 0.000 description 4
- 238000007796 conventional method Methods 0.000 description 3
- 229910001873 dinitrogen Inorganic materials 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000002612 dispersion medium Substances 0.000 description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 2
- 239000012299 nitrogen atmosphere Substances 0.000 description 2
- 238000010298 pulverizing process Methods 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 235000021355 Stearic acid Nutrition 0.000 description 1
- VUAFMBNGAGWGIS-UHFFFAOYSA-K [Y+3].[O-]N=O.[O-]N=O.[O-]N=O Chemical compound [Y+3].[O-]N=O.[O-]N=O.[O-]N=O VUAFMBNGAGWGIS-UHFFFAOYSA-K 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 238000000889 atomisation Methods 0.000 description 1
- GJTDJAPHKDIQIQ-UHFFFAOYSA-L barium(2+);dinitrite Chemical compound [Ba+2].[O-]N=O.[O-]N=O GJTDJAPHKDIQIQ-UHFFFAOYSA-L 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 description 1
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 1
- 239000000292 calcium oxide Substances 0.000 description 1
- 229910002090 carbon oxide Inorganic materials 0.000 description 1
- 229910000420 cerium oxide Inorganic materials 0.000 description 1
- 238000007606 doctor blade method Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000012776 electronic material Substances 0.000 description 1
- 229910001938 gadolinium oxide Inorganic materials 0.000 description 1
- 229940075613 gadolinium oxide Drugs 0.000 description 1
- CMIHHWBVHJVIGI-UHFFFAOYSA-N gadolinium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Gd+3].[Gd+3] CMIHHWBVHJVIGI-UHFFFAOYSA-N 0.000 description 1
- 230000020169 heat generation Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000001307 helium Substances 0.000 description 1
- 229910052734 helium Inorganic materials 0.000 description 1
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- VLAPMBHFAWRUQP-UHFFFAOYSA-L molybdic acid Chemical compound O[Mo](O)(=O)=O VLAPMBHFAWRUQP-UHFFFAOYSA-L 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 238000005121 nitriding Methods 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- QIQXTHQIDYTFRH-UHFFFAOYSA-N octadecanoic acid Chemical compound CCCCCCCCCCCCCCCCCC(O)=O QIQXTHQIDYTFRH-UHFFFAOYSA-N 0.000 description 1
- OQCDKBAXFALNLD-UHFFFAOYSA-N octadecanoic acid Natural products CCCCCCCC(C)CCCCCCCCC(O)=O OQCDKBAXFALNLD-UHFFFAOYSA-N 0.000 description 1
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 239000012188 paraffin wax Substances 0.000 description 1
- RAFRTSDUWORDLA-UHFFFAOYSA-N phenyl 3-chloropropanoate Chemical compound ClCCC(=O)OC1=CC=CC=C1 RAFRTSDUWORDLA-UHFFFAOYSA-N 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 238000010791 quenching Methods 0.000 description 1
- 230000000171 quenching effect Effects 0.000 description 1
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 239000008117 stearic acid Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229940105963 yttrium fluoride Drugs 0.000 description 1
- RBORBHYCVONNJH-UHFFFAOYSA-K yttrium(iii) fluoride Chemical compound F[Y](F)F RBORBHYCVONNJH-UHFFFAOYSA-K 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は窒化アルミニウム焼結体の製造法に関し、詳し
くは粒子径の異なる窒化アルミニウムの（微）粉末を混
合使用することによって、低い焼結温度にて、高密度で
熱伝導性が良好な窒化アルミニウム焼結体を効率よく製
造することのできる方法に関する。Detailed Description of the Invention [Field of Industrial Application] The present invention relates to a method for producing an aluminum nitride sintered body, and more specifically, by mixing and using aluminum nitride (fine) powders with different particle sizes, the present invention can achieve low sintering. The present invention relates to a method for efficiently producing an aluminum nitride sintered body having high density and good thermal conductivity at high temperatures.
〔従来の技術及び発明が解決しようとする課題］近年、
半導体工業の急速な技術進歩により、大規模集積回路（
ＬＳＩ）は、高集積化や高出力化が進行し、それに伴う
発熱量の増大に従来のアルミナ基板では耐えられなくな
ってきている。そのため、アルミナ基板に代わる熱伝導
性の良好な絶縁性基板に対する要求が高まっている。[Problems to be solved by conventional techniques and inventions] In recent years,
Rapid technological advances in the semiconductor industry have led to large-scale integrated circuits (
As LSI (LSI) devices become more highly integrated and output, conventional alumina substrates are no longer able to withstand the accompanying increase in heat generation. Therefore, there is an increasing demand for an insulating substrate with good thermal conductivity to replace the alumina substrate.
このような絶縁性基板に適する素材として、窒化アルミ
ニウム焼結体が知られているが、製造方法が煩雑である
と共に、得られる窒化アルミニウム焼結体の物性が未だ
満足できるものではなかった。例えば、従来から行われ
ている方法は、１〜２μｍの金属アルミニウムを直接窒
化して得られた窒化アルミニウムを焼結する方法が一般
的であるが、この方法では得られる窒化アルミニウム焼
粘体の高密度化は困難であり、また、熱伝導率も６０〜
１００Ｗ／ｍ−に程度にすぎなかった。Aluminum nitride sintered bodies are known as materials suitable for such insulating substrates, but the manufacturing method is complicated and the physical properties of the resulting aluminum nitride sintered bodies are not yet satisfactory. For example, the conventional method is to sinter aluminum nitride obtained by directly nitriding metal aluminum with a thickness of 1 to 2 μm. It is difficult to densify, and the thermal conductivity is 60~60.
It was only about 100 W/m-.
最近になって、特開昭６３−１３４５７０号公報や同６
３−１６６７６５号公報に、新たな窒化アルミニウム焼
結体の製造方法が提案されている。Recently, Japanese Unexamined Patent Publication No. 134570/1983 and 63-134570
No. 3-166765 proposes a new method for producing an aluminum nitride sintered body.
このうち前者の方法は、平均粒径２〜２０１Ｉｍで比表
面積０゜５〜０．３ｒｒｆ／ｇの窒化アルミニウム粉末
を原料とするものであり、得られる窒化アルミニウム焼
結体は性能的にはある程度満足しうるちのである。しか
し、原料が極めて限定されるとともに、焼結温度を高く
しなければならないという大きな問題がある。また、後
者の方法は、焼結用原料を所望形状に成形後、気密性の
容器中で窒素雰囲気下に１７００〜２１００°Ｃの高温
で加熱して焼結体とし、さらに解放系の容器中で窒素気
流中にて１８００〜２１００°Ｃの高温で加熱焼成する
方法である。この方法は、焼結（焼成）温度を高くしな
ければならないという欠点とともに、二段階の焼成処理
を必要とし、実用には不向きなものであった。The former method uses aluminum nitride powder with an average particle size of 2 to 201 Im and a specific surface area of 0.5 to 0.3 rrf/g as a raw material, and the resulting aluminum nitride sintered body has a certain level of performance. Uruchino is satisfied. However, there are major problems in that the raw materials are extremely limited and the sintering temperature must be increased. In the latter method, the raw material for sintering is formed into a desired shape, heated in an airtight container at a high temperature of 1700 to 2100°C under a nitrogen atmosphere to form a sintered body, and then placed in an open container. This is a method of heating and firing at a high temperature of 1800 to 2100°C in a nitrogen stream. This method has the drawback of requiring a high sintering (firing) temperature and requires a two-step firing process, making it unsuitable for practical use.
そこで、本発明者らは簡単な操作で、また低い焼結温度
で処理するだけで、密度が高く熱伝導性の良好な窒化ア
ルミニウム焼結体を製造する方法を開発すべく鋭意研究
を重ねた。Therefore, the present inventors conducted extensive research to develop a method for manufacturing aluminum nitride sintered bodies with high density and good thermal conductivity by simple operations and processing at low sintering temperatures. .
〔課題を解決するための手段］
その結果、原料として平均粒子径０．５〜５μｍの窒化
アルミニウム粉末と平均粒子径０．０１〜０．３μｍの
窒化アルミニウム微粉末とを併用することによって、上
記課題を解決できることを見出した。本発明はかかる知
見に基いて完成したものである。[Means for solving the problem] As a result, by using aluminum nitride powder with an average particle size of 0.5 to 5 μm and aluminum nitride fine powder with an average particle size of 0.01 to 0.3 μm as raw materials, the above-mentioned solution can be achieved. I discovered that I could solve the problem. The present invention was completed based on this knowledge.
すなわち、本発明は（Ａ）平均粒子径０．５〜５μｍの
窒化アルミニウム粉末、（Ｂ）平均粒子径０，０１〜０
．３μｍの窒化アルミニウム微粉末および（Ｃ）焼結助
剤を混合して成形し、得られた成形体を非酸化性雰囲気
下で焼結することを特徴とする窒化アルミニウム焼結体
の製造法を提供するものである。That is, the present invention uses (A) aluminum nitride powder with an average particle size of 0.5 to 5 μm, (B) an average particle size of 0.01 to 0.
．． A method for producing an aluminum nitride sintered body, which comprises mixing and molding a 3 μm aluminum nitride fine powder and (C) a sintering aid, and sintering the resulting molded body in a non-oxidizing atmosphere. This is what we provide.
本発明の製造法では、上述の如く原料として（Ａ）、（
Ｂ）二種類の平均粒子径の異なる窒化アルミニウム（微
）粉末を用いることが必要である。In the production method of the present invention, as mentioned above, the raw materials are (A), (
B) It is necessary to use two types of aluminum nitride (fine) powders with different average particle sizes.
ここで、（Ａ）成分である窒化アルミニウム粉末として
は、平均粒子径０．５〜５μｍ、好ましくは０．５〜２
μｍのものが用いられる。この窒化アルミニウム粉末は
、各種公知の方法によって得られるものを充当すればよ
く、特に制限はない。Here, the average particle size of the aluminum nitride powder as component (A) is 0.5 to 5 μm, preferably 0.5 to 2 μm.
μm is used. This aluminum nitride powder may be obtained by various known methods, and is not particularly limited.
様々な方法によって得られる窒化アルミニウムをそのま
ま、あるいはこれをさらに粉砕したものが用いられる。Aluminum nitride obtained by various methods can be used as it is, or it can be further pulverized.
ここで上述の平均粒子径の範囲に粉砕するには、これも
また各種の手法によることができるが、例えば、アトマ
イズ法、液体急冷法あるいはジェットミル、ボールミル
、スタンプミル等の従来から一般に行われている機械的
粉砕法などによればよい。このような窒化アルミニウム
粉末には、若干の不純物が混入したものであっても使用
上支障はないが、通常は酸素含有量が１重量％以下、金
属不純物合計含有量が１１００ｐｐ以下ものが好ましい
。Here, pulverization to the above-mentioned average particle size range can also be done by various methods, but for example, conventional methods such as an atomization method, a liquid quenching method, a jet mill, a ball mill, a stamp mill, etc. are commonly used. Mechanical pulverization methods may be used. Such aluminum nitride powder may contain a small amount of impurities without any problem in use, but it is usually preferable that the oxygen content be 1% by weight or less and the total metal impurity content be 1100 pp or less.
一方、ＣＢ）成分である窒化アルミニウム微粉末として
は、平均粒子径０．０１〜０．３μｍ、好ましくは０．
０５〜０．２μｍのものが用いられる。On the other hand, the average particle size of the aluminum nitride fine powder which is the component CB) is 0.01 to 0.3 μm, preferably 0.01 to 0.3 μm.
05 to 0.2 μm is used.
この窒化アルミニウム微粉末は、様々な方法によって調
製することが可能であるが、例えば、高周波プラズマ法
、直流アークプラズマ法、アークプラズマジェット法、
ハイブリッドプラズマ法等の従来から行われているプラ
ズマ法によって得ることができる。本発明に用いる窒化
アルミニウム微粉末には、若干の不純物が混入したもの
であってもよいが、通常は酸素含有量が２．０重量％以
下、金属不純物合計含有量が５０ｐｐｍ以下ものが好ま
しい。This fine aluminum nitride powder can be prepared by various methods, such as high frequency plasma method, DC arc plasma method, arc plasma jet method,
It can be obtained by a conventional plasma method such as a hybrid plasma method. Although the aluminum nitride fine powder used in the present invention may contain some impurities, it is usually preferable that the oxygen content is 2.0% by weight or less and the total metal impurity content is 50 ppm or less.
本発明の製造法では、原料として上記（Ａ）。In the production method of the present invention, the above (A) is used as a raw material.
（Ｂ）両成分を用いることが必要であり、ここで（Ａ）
成分のみでは、焼結温度が高くなるばかりか、高密度の
焼結体が得られ難いという不都合が生じ、また（Ｂ）成
分のみでは、原料微粉末が高価であるため安価な焼結体
が得られないばかりか、原料の酸素含有量が高く、結果
として熱伝導率の高い焼結体が得られないという不都合
がある。(B) It is necessary to use both components, where (A)
Using component (B) alone not only increases the sintering temperature but also makes it difficult to obtain a high-density sintered body, and using only component (B) makes it difficult to produce an inexpensive sintered body because the raw material fine powder is expensive. Not only is this not possible, but the oxygen content of the raw material is high, resulting in the inconvenience that a sintered body with high thermal conductivity cannot be obtained.
上記（Ａ）、（Ｂ）両成分を併用するにあたっては、両
成分の使ＪｌｆｉＰＪ合は特に制限はなく、状況に応じ
て適宜選定すればよいが、好ましくは（Ａ）成分である
平均粒子径０．５〜５μｍの窒化アルミニウム粉末９９
．５〜５０重量％、（Ｂ）成分である平均粒子径０．０
１〜０．３μｍの窒化アルミニウム微粉末０．５〜５０
重量％であり、特に好ましくは（Ａ）成分９９〜７０９
〜７０重量）成分１〜３０重量％の範囲である。When using both components (A) and (B) above, there is no particular restriction on the use of both components, and they may be selected as appropriate depending on the situation, but preferably the average particle diameter of component (A) 0.5-5 μm aluminum nitride powder 99
．． 5 to 50% by weight, average particle diameter of component (B) 0.0
1-0.3 μm aluminum nitride fine powder 0.5-50
% by weight, particularly preferably component (A) 99 to 709
~70% by weight) component ranges from 1 to 30% by weight.
本発明の製造法では、上記原料成分とともに、（Ｃ）成
分として焼結助剤を加える。この焼結助剤としては、従
来からこの種の焼結体の製造に用いられている各種のも
のを用いることができ、例えば、酸化イツトリウム、酸
化ランタン、酸化セリウム、酸化ガドリニウム等の希土
類酸化物をはじめ、酸化カルシウム、酸化ジルコニウム
、フッ化イツトリウム、亜硝酸カルシウム、亜硝酸バリ
ウム、亜硝酸イツトリウムなどを好適に使用できる。こ
の（Ｃ）成分である焼結助剤の配合割合は、各種の条件
に応じて適宜定めればよいが、好ましくは前述の（Ａ）
、（Ｂ）両成分の合計量に対して０．２〜１０重量％の
割合、特に好ましくは０．５〜６重量％とする。ここで
、焼結助剤の配合割合が少なすぎると、焼結密度が充分
に高くならない場合があり、逆にあまり多すぎても得ら
れる焼結体の熱伝導性が低下するおそれがある。また、
この焼結助剤の粒子径については、用いる焼結助剤の種
類、その配合割合等により異なるが、通常は平均粒子径
０．１〜１．０μｍ程度のものが好ましい。In the manufacturing method of the present invention, a sintering aid is added as component (C) along with the above raw material components. As this sintering aid, various kinds of materials conventionally used in the production of this type of sintered body can be used, such as rare earth oxides such as yttrium oxide, lanthanum oxide, cerium oxide, and gadolinium oxide. In addition, calcium oxide, zirconium oxide, yttrium fluoride, calcium nitrite, barium nitrite, yttrium nitrite, and the like can be suitably used. The blending ratio of the sintering aid, which is component (C), may be determined as appropriate depending on various conditions, but it is preferable to use the above-mentioned (A).
, (B) in a proportion of 0.2 to 10% by weight, particularly preferably 0.5 to 6% by weight, based on the total amount of both components. Here, if the blending ratio of the sintering aid is too small, the sintered density may not be sufficiently high, whereas if it is too large, the thermal conductivity of the obtained sintered body may be reduced. Also,
The particle diameter of this sintering aid varies depending on the type of sintering aid used, its blending ratio, etc., but it is usually preferable to have an average particle diameter of about 0.1 to 1.0 μm.
本発明の製造法では、上記の（Ａ）、（Ｂ）、（ｃ）成
分を所定割合で混合して成形するが、さらにこの際に、
所望により成形助剤（バインダーなど）。In the manufacturing method of the present invention, the above components (A), (B), and (c) are mixed in a predetermined ratio and molded.
Molding aids (binder, etc.) if desired.
分散媒体を適量配合することもできる。この成形助剤と
しては、モリブデン酸などのほか、パラフィン、ポリビ
ニルアルコール、ポリビニルブチラール、ステアリン酸
など公知のものを用いることができる。また、分散媒体
としては水、アルコール、炭化水素類あるいはこれらの
混合物が好適に用いられる。An appropriate amount of a dispersion medium can also be blended. As this molding aid, in addition to molybdic acid, known ones such as paraffin, polyvinyl alcohol, polyvinyl butyral, and stearic acid can be used. Moreover, water, alcohol, hydrocarbons, or a mixture thereof is preferably used as the dispersion medium.
本発明の製造法では、これら各成分を充分に混合した後
に、成形して所定形状の成形体を作製する。成形方法と
しては、ボールミル等によす充分混合されたものを、必
要により乾燥した後、金型成形法、静水圧成形法、ドク
ターブレード法などを採用することができる。続いてこ
の成形体を非酸化性雰囲気下、即ち真空あるいは窒素ガ
ス、水素ガス、−酸化炭素ガス、アルゴンガス、ヘリウ
ムガス等の雰囲気下で焼結する。焼結温度は特に制限な
ないが、一般には１５００〜２１００°Ｃの範囲で適宜
定めればよい。また、この焼結の際の他の条件としては
、特にないが、通常は常圧にて、成形体の形状や大きさ
に応じた時間焼結を行えばよい。In the manufacturing method of the present invention, these components are thoroughly mixed and then molded to produce a molded article of a predetermined shape. As a molding method, the mixture may be thoroughly mixed using a ball mill or the like, dried if necessary, and then a mold molding method, an isostatic molding method, a doctor blade method, or the like can be employed. Subsequently, this compact is sintered in a non-oxidizing atmosphere, that is, in a vacuum or in an atmosphere of nitrogen gas, hydrogen gas, -carbon oxide gas, argon gas, helium gas, or the like. The sintering temperature is not particularly limited, but it may generally be set appropriately within the range of 1500 to 2100°C. Further, there are no other conditions for this sintering, but the sintering may normally be performed at normal pressure for a time depending on the shape and size of the compact.
本発明の製造法では、このような焼結処理を行えば、優
れた性状の窒化アルミニウム焼結体が得られるが、さら
に必要に応じて、窒素雰囲気あるいは窒化物容器中で焼
成を行うこともできる。この焼成を行うことにより、焼
結体中の酸素含有量を低減させて、該焼結体の熱伝導性
を一層高めることが可能である。In the manufacturing method of the present invention, an aluminum nitride sintered body with excellent properties can be obtained by performing such a sintering process, but if necessary, the sintering can also be performed in a nitrogen atmosphere or in a nitride container. can. By performing this firing, it is possible to reduce the oxygen content in the sintered body and further improve the thermal conductivity of the sintered body.
次に本発明を実施例および比較例により、さらに詳しく
説明する。Next, the present invention will be explained in more detail with reference to Examples and Comparative Examples.
実施例１
市販の窒化アルミニウム粉末（平均粒子径１．０μｍ）
に、直流アークプラズマを用いて製造した窒化アルミニ
ウム微粉末（平均粒子径０．１μｍ。Example 1 Commercially available aluminum nitride powder (average particle size 1.0 μm)
Fine aluminum nitride powder (average particle size 0.1 μm) was produced using DC arc plasma.
酸素含有Ｎ２．０重量％、金属不純物合計５０ｐｐｍ以
下）を、前者：後者＝９６：４（重量比）の割合で加え
、さらに焼結助剤として酸化イツトリウムを、前記窒化
アルミニウム粉末と窒化アルミニウム微粉末の合計量に
対して３重量％の割合で加えて混合し、成形した。2.0% by weight of oxygen-containing N, 50 ppm or less of metal impurities in total) was added at a ratio of 96:4 (weight ratio), and yttrium oxide was added as a sintering aid to the aluminum nitride powder and aluminum nitride fine powder. It was added in a proportion of 3% by weight based on the total amount of powder, mixed, and molded.
次に、得られた成形体を窒素ガス雰囲気中で、常圧、１
５００°Ｃの条件にて３時間焼結処理を行った。Next, the obtained molded body was placed in a nitrogen gas atmosphere at normal pressure for 1
Sintering treatment was performed at 500°C for 3 hours.
得られた焼結体は、密度が３．２６ ｇ ／ｃ４であり
、１００％理論密度に達していることがわかった。また
、この焼結体の熱伝導率は２００Ｗ／ｍ−にであった。It was found that the obtained sintered body had a density of 3.26 g/c4, reaching 100% of the theoretical density. Further, the thermal conductivity of this sintered body was 200 W/m-.
実施例２
実施例１において、窒化アルミニウム粉末と窒化アルミ
ニウム微粉末との混合割合を、９８：２（重量比）とし
たこと以外は、実施例１と同様な操作を行った。Example 2 The same operation as in Example 1 was performed except that the mixing ratio of aluminum nitride powder and aluminum nitride fine powder was 98:2 (weight ratio).
得られた焼結体は、密度が３．２３ｇ／ｃ＋ｆｌであり
、９９％理論密度に達していることがわかった。It was found that the obtained sintered body had a density of 3.23 g/c+fl, reaching 99% of the theoretical density.
また、この焼結体の熱伝導率は１６０Ｗ／ｍ−にであっ
た。Further, the thermal conductivity of this sintered body was 160 W/m-.
実施例３
実施例１において、窒化アルミニウム粉末と窒化アルミ
ニウム微粉末との混合割合を、９０：１０（重量比）と
したこと以外は、実施例１と同様な操作を行った。Example 3 The same operation as in Example 1 was performed except that the mixing ratio of aluminum nitride powder and aluminum nitride fine powder was 90:10 (weight ratio).
得られた焼結体は、密度が３．２４ ｇ ／ｃ１１１で
あり、９９％理論密度に達していることがわかった。It was found that the obtained sintered body had a density of 3.24 g/c111, reaching 99% of the theoretical density.
また、この焼結体の熱伝導率は１８０Ｗ／ｍ、にであっ
た。Further, the thermal conductivity of this sintered body was 180 W/m.
実施例４
実施例１において、窒化アルミニウム粉末と窒化アルミ
ニウム微粉末との混合割合を、８０：２０（重量比）と
したこと以外は、実施例１と同様な操作を行った。Example 4 The same operation as in Example 1 was performed except that the mixing ratio of aluminum nitride powder and aluminum nitride fine powder was 80:20 (weight ratio).
得られた焼結体は、密度が３．２３ ｇ ／ｃｄであり
、９９％理論密度に達していることがわかった。It was found that the obtained sintered body had a density of 3.23 g/cd, reaching 99% of the theoretical density.
また、この焼結体の熱伝導率は１７５ Ｗ／ｍ−にであ
った。Further, the thermal conductivity of this sintered body was 175 W/m-.
比較例１
実施例１と同じ市販の窒化アルミニウム粉末（平均粒子
径１．０μｍ）に、焼結助剤として実施例１と同じ酸化
イツトリウムを、３重量％の割合で加えて混合し、成形
した。Comparative Example 1 The same yttrium oxide as in Example 1 was added as a sintering aid to the same commercially available aluminum nitride powder (average particle size 1.0 μm) as in Example 1 at a ratio of 3% by weight, and the mixture was molded. .
次に、得られた成形体を窒素ガス雰囲気中で、常圧、１
５００°Ｃの条件にて３時間焼結処理を行った。Next, the obtained molded body was placed in a nitrogen gas atmosphere at normal pressure for 1
Sintering treatment was performed at 500°C for 3 hours.
得られた焼結体は、密度が２．６５ ｇ ／ｃ４であり
、理論密度の８１％に達しただけであった。また、この
焼結体の熱伝導率は８２Ｗ／ｍ−にであった。The obtained sintered body had a density of 2.65 g/c4, which was only 81% of the theoretical density. Further, the thermal conductivity of this sintered body was 82 W/m-.
叙上の如く、本発明の製造法によれ・ば、簡単な操作で
、また低い焼結温度で、密度が高くしかも熱伝導性の良
好な窒化アルミニウム焼結体を製造することができる。As described above, according to the production method of the present invention, an aluminum nitride sintered body having high density and good thermal conductivity can be produced with simple operations and at a low sintering temperature.
本発明の製造法は、操作が簡単であるとともに、焼結の
際の温度が低いため運転コストが安価であり、また原料
の入手が比較的容易であるため、工業的に極めて有利で
ある。The production method of the present invention is industrially extremely advantageous because it is easy to operate, the operating cost is low because the temperature during sintering is low, and raw materials are relatively easy to obtain.
また、本発明の製造法で製造される窒化アルミニウム焼
結体は、高密度であってしかも熱伝導性が良好なもので
あるため、高集積化された大規模集積回路の絶縁性基板
をはじめとする電子材料、さらには各種構造材料等に幅
広くかつ有効な利用が期待される。In addition, the aluminum nitride sintered body manufactured by the manufacturing method of the present invention has a high density and good thermal conductivity, so it can be used for insulating substrates of highly integrated large-scale integrated circuits, etc. It is expected that it will find wide and effective use in electronic materials and various structural materials.
Claims (2)
ウム粉末，（Ｂ）平均粒子径０．０１〜０．３μｍの窒
化アルミニウム微粉末および（Ｃ）焼結助剤を混合して
成形し、得られた成形体を非酸化性雰囲気下で焼結する
ことを特徴とする窒化アルミニウム焼結体の製造法。(1) (A) Aluminum nitride powder with an average particle size of 0.5 to 5 μm, (B) Fine aluminum nitride powder with an average particle size of 0.01 to 0.3 μm, and (C) Sintering aid are mixed and molded. and sintering the obtained compact in a non-oxidizing atmosphere.
ウム粉末９９．５〜５０重量％，（Ｂ）平均粒子径０．
０１〜０．３μｍの窒化アルミニウム微粉末０．５〜５
０重量％および（Ｃ）焼結助剤を前記（Ａ）窒化アルミ
ニウム粉末と（Ｂ）窒化アルミニウム微粉末の合計に対
して０．２〜１０重量％の割合で混合してなる請求項１
記載の製造法。(2) (A) 99.5-50% by weight of aluminum nitride powder with an average particle size of 0.5-5 μm, (B) 0.5-50% by weight of aluminum nitride powder with an average particle size of 0.5-5 μm.
01-0.3 μm aluminum nitride fine powder 0.5-5
0% by weight and (C) a sintering aid mixed in a proportion of 0.2 to 10% by weight based on the total of the (A) aluminum nitride powder and (B) fine aluminum nitride powder.
Manufacturing method described.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63207264A JPH0259473A (en) | 1988-08-23 | 1988-08-23 | Production of aluminum nitride sintered body |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63207264A JPH0259473A (en) | 1988-08-23 | 1988-08-23 | Production of aluminum nitride sintered body |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH0259473A true JPH0259473A (en) | 1990-02-28 |
Family
ID=16536913
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP63207264A Pending JPH0259473A (en) | 1988-08-23 | 1988-08-23 | Production of aluminum nitride sintered body |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0259473A (en) |
-
1988
- 1988-08-23 JP JP63207264A patent/JPH0259473A/en active Pending
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