JPS63277572A - Production of sintered aluminum nitride - Google Patents
Production of sintered aluminum nitrideInfo
- Publication number
- JPS63277572A JPS63277572A JP62110809A JP11080987A JPS63277572A JP S63277572 A JPS63277572 A JP S63277572A JP 62110809 A JP62110809 A JP 62110809A JP 11080987 A JP11080987 A JP 11080987A JP S63277572 A JPS63277572 A JP S63277572A
- Authority
- JP
- Japan
- Prior art keywords
- aluminum nitride
- sintered body
- weight
- container
- sintered
- 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 description 28
- 238000004519 manufacturing process Methods 0.000 title claims description 8
- 239000000843 powder Substances 0.000 claims abstract description 25
- 150000001875 compounds Chemical class 0.000 claims abstract description 17
- 239000002245 particle Substances 0.000 claims abstract description 17
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 16
- 239000001301 oxygen Substances 0.000 claims abstract description 16
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 16
- 239000007789 gas Substances 0.000 claims abstract description 12
- 239000012535 impurity Substances 0.000 claims abstract description 11
- 229910052727 yttrium Inorganic materials 0.000 claims abstract description 11
- 229910052761 rare earth metal Inorganic materials 0.000 claims abstract description 10
- 230000001590 oxidative effect Effects 0.000 claims abstract description 6
- 229910052712 strontium Inorganic materials 0.000 claims abstract description 5
- 238000005452 bending Methods 0.000 claims abstract description 4
- 229910052746 lanthanum Inorganic materials 0.000 claims abstract description 4
- 229910052791 calcium Inorganic materials 0.000 claims abstract description 3
- 238000010304 firing Methods 0.000 claims description 23
- -1 Ca and Sr Chemical class 0.000 claims description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 abstract description 7
- 238000000465 moulding Methods 0.000 abstract description 7
- 239000011230 binding agent Substances 0.000 abstract description 5
- 229910052593 corundum Inorganic materials 0.000 abstract description 4
- 229910001845 yogo sapphire Inorganic materials 0.000 abstract description 4
- 238000001354 calcination Methods 0.000 abstract 2
- 239000000203 mixture Substances 0.000 abstract 2
- 238000005245 sintering Methods 0.000 description 28
- 239000000654 additive Substances 0.000 description 15
- 238000011156 evaluation Methods 0.000 description 10
- 230000000996 additive effect Effects 0.000 description 9
- 239000002994 raw material Substances 0.000 description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 7
- 229910052799 carbon Inorganic materials 0.000 description 7
- 238000000034 method Methods 0.000 description 6
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 229910001873 dinitrogen Inorganic materials 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 2
- 238000005238 degreasing Methods 0.000 description 2
- 238000000280 densification Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000005121 nitriding Methods 0.000 description 2
- 238000010298 pulverizing process Methods 0.000 description 2
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 229910052692 Dysprosium Inorganic materials 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- 229910002090 carbon oxide Inorganic materials 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 150000002222 fluorine compounds Chemical class 0.000 description 1
- 239000003779 heat-resistant material Substances 0.000 description 1
- 238000007731 hot pressing Methods 0.000 description 1
- 150000004679 hydroxides Chemical class 0.000 description 1
- 239000012212 insulator Substances 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000011812 mixed powder Substances 0.000 description 1
- 238000003947 neutron activation analysis Methods 0.000 description 1
- 150000002823 nitrates Chemical class 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 150000003891 oxalate salts Chemical class 0.000 description 1
- 238000013001 point bending Methods 0.000 description 1
- 238000001272 pressureless sintering Methods 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 150000003748 yttrium compounds Chemical class 0.000 description 1
Abstract
Description
【発明の詳細な説明】
〔発明の目的〕
（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方法に関する
。DETAILED DESCRIPTION OF THE INVENTION [Object of the Invention] (Field of Industrial Application) The present invention relates to a method for producing an aluminum nitride sintered body.
（従来の技術）
窒化アルミニウム（ＡｉＮ）は高温まで強度低下が少な
く、化学的耐性にも優れているため、耐熱材料として用
いられる一方、その高温伝導性、高電気絶縁性を利用し
て半導体装置の放熱板材料、回路基板用絶縁体材料とし
ても有望視されている。(Prior art) Aluminum nitride (AiN) has little strength loss even at high temperatures and has excellent chemical resistance, so it is used as a heat-resistant material. It is also seen as a promising material for heat sinks and insulators for circuit boards.
こうした窒化アルミニウムは常圧下では融点を持たず、
ｚｓｏｏ℃以上の高温で分解するため、薄膜などの用
途を除いては焼結体として用いられる。Such aluminum nitride does not have a melting point under normal pressure,
Since it decomposes at high temperatures above zsoo°C, it is used as a sintered body except for applications such as thin films.
かかる窒化アルミニウム焼結体は通常、窒化アルミニウ
ム粉末を成形、焼結して得られる。Such an aluminum nitride sintered body is usually obtained by molding and sintering aluminum nitride powder.
しかしながら１粒径０．５−以上のＡｉＮ粉末を単独で
用いた場合は焼結性が良好でないために、ホットプレス
法による以外には無添加では緻密な焼結体を得ることは
困難である。However, when AiN powder with a grain size of 0.5- or more is used alone, the sinterability is not good, so it is difficult to obtain a dense sintered body without additives other than by hot pressing. .
このようなことから、常圧で焼結する場合には。For this reason, when sintering at normal pressure.
通常、焼結体の高密度化を目的として、焼結助剤として
希土類酸化物、アルカリ土類金属酸化物等を添加し、カ
ーボン容器またはＢＮを塗布したカーボン容器または７
４Ｎ粉末のつめ物中で焼結することが一般に行なわれて
いる。高熱伝導率化のためには、原料粉の酸素量が少な
いことが必要とされる。しかしながら粒径の粗い粉は、
粉砕すると酸素量が増加するため、粉砕することなしに
、そのまま焼成すると、上記容器中では緻密化しない。Usually, for the purpose of increasing the density of the sintered body, rare earth oxides, alkaline earth metal oxides, etc. are added as sintering aids, and carbon containers or BN-coated carbon containers or 7
Sintering in a 4N powder filler is commonly practiced. In order to achieve high thermal conductivity, it is necessary that the amount of oxygen in the raw material powder is small. However, coarse-grained powder
Since pulverization increases the amount of oxygen, if the material is fired as is without pulverization, it will not become densified in the container.
酸素量が少なく１粒径の粗い原料粉を用いても緻密化す
る焼成条件が必要である。また、希土類酸化物を添加し
、カーボン容器中で焼成した焼結体は、表面にＡｆｆｉ
Ｎでない化合物が生成する。また、アルカリ土類金属酸
化物を添加し、カーボン容器中で焼成した焼結体は、変
形するなど焼き上がりの状態が良好ではない。Firing conditions are required that provide densification even when using coarse raw material powder with a small amount of oxygen and a single grain size. In addition, the sintered body added rare earth oxide and fired in a carbon container has Affi on the surface.
A compound that is not N is produced. Moreover, the sintered body added with an alkaline earth metal oxide and fired in a carbon container is not in a good condition after being fired, such as deformation.
（発明が解決しようとする問題点）
ている。しかしながら、カーボン容器またはＢＮを塗布
したカーボン容器またはＡＱＮ粉末のつめ物中による焼
成では、Ｈｌ、密化しにくいため、高強度も得られない
。(Problem that the invention seeks to solve) However, when firing in a carbon container, a carbon container coated with BN, or a filling of AQN powder, high strength cannot be obtained because Hl is difficult to densify.
本発明は、以上の点を考慮してなされたもので。The present invention has been made in consideration of the above points.
緻密で焼き上がり状態の良好な窒化アルミニウム焼結体
を提供することを目的とする。The purpose of the present invention is to provide an aluminum nitride sintered body that is dense and has a good baked condition.
（問題点を解決するための手段及び作用）本発明者等は
上記目的を達成すべく窒化アルミニウム粉末に添加する
焼結助剤や焼結条件と、得られた焼結体の密度及び抗折
強度との関係について実験・検討を進めた結果、以下に
示す新規事項を発見し１本発明を完成するに至った。(Means and effects for solving the problem) In order to achieve the above object, the present inventors have investigated the sintering aid added to the aluminum nitride powder, the sintering conditions, and the density and bending resistance of the obtained sintered body. As a result of conducting experiments and studies regarding the relationship with strength, we discovered the following new matter and completed the present invention.
すなわち、焼結助剤としてイツトリウム化合物をＡｆｆ
ｉＮ粉末に添加し、（１−０）ガス雰囲気をつくり出す
容器中で焼成したところ、焼き上がり状態の良好な高密
度で、高強度を有する窒化アルミニウム焼結体が得られ
るという事実をみいだした。That is, using yttrium compound as a sintering aid
We have discovered that when added to iN powder and fired in a container that creates a (1-0) gas atmosphere, a sintered aluminum nitride body with good firing quality, high density, and high strength can be obtained. .
この効果は他のＩＩａ族化合物（Ｓｒ、 Ｙ）、ＩＩａ
ＩＩａ族化合物ａ 、Ｂａ 、Ｓｒ等）および希土類元
素（Ｌａ、Ｃｅ、Ｄｙ、Ｃｏ等）でも同様に認められた
。This effect is similar to other group IIa compounds (Sr, Y), IIa
The same phenomenon was observed in Group IIa compounds (a, Ba, Sr, etc.) and rare earth elements (La, Ce, Dy, Co, etc.).
この事実に基づいて高密度化を達成する最適条件を種々
検討した結果が本発明であり。The present invention is the result of various studies on optimal conditions for achieving high density based on this fact.
ａ）不純物酸素量が５重量％以下であり、平均粒径が０
．０５〜ｉｏ、である窒化アルミニウム粉末と。a) The amount of impurity oxygen is 5% by weight or less, and the average particle size is 0.
．． 05~io, and aluminum nitride powder.
Ｃａ、 ＳｒなどのＩＩａ族、Ｙ、ＬａなどのＩＩａ族
及び希土類元素の重量換算で０．０１〜１５重量％の、
ＩＩａＩＩａ族化合物Ｉ［［ａ族化合物および／又は
希土類元素化合物とを混合したのち成形した成形体をｂ
） ＡＩＩ！、０．製容器中もしくは、Ａｌ２Ｏ３焼
結体、１．０３粉末で焼成中に（Ａ＋１！−０）ガス雰
囲気をつくり出し
Ｃ）非酸化性ガス雰囲気、１５５０〜２０５０℃で焼成
することを特徴とした窒化アルミニウム焼結体の製造方
法である。0.01 to 15% by weight of group IIa elements such as Ca and Sr, group IIa elements such as Y and La, and rare earth elements;
IIa Group IIa compound I
) AII! ,0. An aluminum nitride characterized by creating a (A+1!-0) gas atmosphere in a container or during firing with an Al2O3 sintered body or 1.03 powder, and C) firing at a temperature of 1550 to 2050°C in a non-oxidizing gas atmosphere. This is a method for manufacturing a sintered body.
この様な方法で得られた窒化アルミニウム焼結体は、表
面状態は粗でなく、変形することもなく。The aluminum nitride sintered body obtained by this method does not have a rough surface and does not deform.
相対密度８５％以上、抗折強度２０ｋｇｃｓｇ−”以上
を有する。It has a relative density of 85% or more and a bending strength of 20 kgcsg-'' or more.
本発明の製造方法は、窒化アルミニウム原料粉末の純度
および平均粒径、焼結助剤、焼結容器、焼成時間および
焼成雰囲気を骨子とするものである。The main points of the production method of the present invention are the purity and average particle size of the aluminum nitride raw material powder, sintering aid, sintering container, firing time, and firing atmosphere.
主成分である窒化アルミニウム原料粉末としては、焼結
性を考慮して酸素を５重量％以下１．平均粒径が０．０
５〜１０−のものを使用する。In consideration of sinterability, the aluminum nitride raw material powder, which is the main component, contains 5% by weight or less of oxygen. Average particle size is 0.0
Use one with a weight of 5 to 10.
添加物としてはＣａ、ＳＦなどのＩＩａ族化合物、Ｙ、
ＬａなどのＩＩａ族化合物および希土類元素化合物（特
にイツトリウム化合物が好ましい）を用いる。Additives include Ca, IIa group compounds such as SF, Y,
Group IIa compounds such as La and rare earth element compounds (yttrium compounds are particularly preferred) are used.
前述の化合物としては、酸化物、窒化物、フッ化物、酸
フッ化物、酸窒化物、もしくは焼成によりこれらの化合
物となる物質が最適である。焼成によって例えば酸化物
となる物質とし・では、これら元素の炭酸塩、硝酸塩、
シュウ酸塩、水酸化物などをあげることができる。The above-mentioned compounds are optimally oxides, nitrides, fluorides, oxyfluorides, oxynitrides, or substances that become these compounds upon firing. For example, substances that become oxides when fired are carbonates, nitrates,
Examples include oxalates and hydroxides.
希土類元素化合物等の添加は、希土類元素等の元素の重
量換算で０．０１〜１５重量％の範囲で添加する。The rare earth element compound and the like are added in an amount of 0.01 to 15% by weight in terms of the weight of the element such as the rare earth element.
燐酸容器に関しては、焼成中に（ｉ−０）ガス雰囲気を
つくり出す容器を用いる。この様な焼成容器としては、
容器全体がＡらＯｌの物、容器全体がＡＱ、Ｏ□製で試
料を設置する箇所にＡｇＮ板、ＢＮ板、Ｗ板等を敷いた
もの等を用いることができる。Regarding the phosphoric acid container, a container that creates an (i-0) gas atmosphere during firing is used. As such a firing container,
It is possible to use a container in which the entire container is made of A or Ol, or a container in which the entire container is made of AQ or O□ and where the sample is placed is lined with an AgN plate, BN plate, W plate, etc.
焼結時間については、前述の如くの（１−０）ガス雰囲
気が得られない焼成容器を用いた場合は。Regarding the sintering time, if a sintering container in which the (1-0) gas atmosphere as described above cannot be obtained is used.
３０分〜２時間の短時間の焼成によっても、表面状態が
粗である。また変形する等の窒化アルミニウム焼結体が
得られるが、前述の如くの（Ａｌ−０）ガス雰囲気が得
られる焼成容器中で焼成した場合は。Even after firing for a short time of 30 minutes to 2 hours, the surface condition remains rough. Furthermore, an aluminum nitride sintered body that is deformable can be obtained when fired in a firing vessel that provides an (Al-0) gas atmosphere as described above.
焼結温度にもよるが、目的温度まで上げすぐに冷却した
としても、窒化アルミニウム焼結体の緻密化は可能であ
る。より好ましくは、３０分以上である。Although it depends on the sintering temperature, it is possible to densify the aluminum nitride sintered body even if the temperature is raised to the target temperature and immediately cooled. More preferably, it is 30 minutes or more.
焼成温度については、 １５５０〜２０５０℃が好まし
い。Regarding the firing temperature, 1550 to 2050°C is preferable.
１５５０℃より低温で焼成すると、原料粉末の粒径。When fired at a temperature lower than 1550°C, the particle size of the raw material powder.
酸素量にもよるが緻密な焼結体が得られない、また２０
５０℃より高温で焼成すると、ＡＸＮ自体の蒸気圧が高
くなり、緻密化が困難になる。焼成温度はより好ましく
は１６００〜１９５０℃である。Depending on the amount of oxygen, a dense sintered body cannot be obtained;
When fired at a temperature higher than 50° C., the vapor pressure of AXN itself increases, making densification difficult. The firing temperature is more preferably 1600 to 1950°C.
焼成雰囲気は、窒素ガス、水素ガス、−酸化炭素、アル
ゴン等の群から選ばれる１種または２種以上の非酸化性
雰囲気が好ましい、なお焼結は。The sintering atmosphere is preferably one or more non-oxidizing atmospheres selected from the group of nitrogen gas, hydrogen gas, -carbon oxide, argon and the like.
減圧、加圧及び常圧を含む雰囲気圧下で行なう。It is carried out under atmospheric pressure including reduced pressure, increased pressure and normal pressure.
次いで本発明の窒化アルミニウム焼結体の製造方法の一
例を以下に述べる。Next, an example of the method for manufacturing the aluminum nitride sintered body of the present invention will be described below.
まず、Ａ、ＩＮ粉末に焼結添加物として希土類元素化合
物を所定量添加したのちボールミル等を用いて混合する
。焼結には常圧焼結法を使用する。First, a predetermined amount of a rare earth element compound as a sintering additive is added to the A and IN powders, and then mixed using a ball mill or the like. The pressureless sintering method is used for sintering.
この場合、混合粉末にバインダーを加え、混練、造粒、
整粒を行なったのち成形する。成形法としては、金型プ
レス、静水圧プレス或いはシート成形などが適用できる
。続いて、成形体を非酸化性雰囲気中１例えば窒素ガス
気流中で加熱してバインダーを除去したのち常圧焼結す
る。焼結温度は１５５０〜２０５０℃に設定する。In this case, a binder is added to the mixed powder, kneaded, granulated,
After grading, it is molded. As a molding method, a mold press, isostatic press, sheet molding, etc. can be applied. Subsequently, the molded body is heated in a non-oxidizing atmosphere, for example, in a nitrogen gas stream to remove the binder, and then sintered under normal pressure. The sintering temperature is set at 1550-2050°C.
（実施例）
失立涯よ
不純物としての酸素を１．３重量％含有し、平均粒径が
２．１−のＡ旦Ｎ粉末に、添加物として平均粒径０．９
４のＹ２Ｏ，をイツトリウム元素の重量換算７２．５重
量％添加し、ボールミルを用いて混合を行ない原料を調
整した。ついで、この原料に有機系バインダーを４重量
％添加して造粒したのち５００ｋｇ／ｄ （７）圧力で
プレス成形しテ４４ Ｘ ３４ Ｘ ５．２閣の圧粉体
とした。この圧粉体を窒素ガス′＃囲気中で７００℃ま
で加熱してバインダーを除去した。(Example) An additive containing 1.3% by weight of oxygen as an impurity and having an average particle size of 2.1% was added as an additive.
4 was added in an amount of 72.5% by weight in terms of the weight of yttrium element, and mixed using a ball mill to prepare a raw material. Next, 4% by weight of an organic binder was added to this raw material and granulated, followed by press molding at a pressure of 500 kg/d (7) to obtain a green compact with a size of 44 x 34 x 5.2 mm. The compact was heated to 700° C. in a nitrogen gas atmosphere to remove the binder.
更に、ＢＮ粉末を塗布したＡ、ＩＮ板を底抜としてひい
たアルミナ製容器（焼成用容器Ａ）に脱脂体を収容した
。Further, the degreased body was housed in an alumina container (firing container A) made of an A and IN plate coated with BN powder and made with a hollow bottom.
この容器を用い窒素ガス雰囲気中（１気圧）１８５０℃
、２時間の条件で常圧焼結した。得られたＡユＮ焼結体
の密度を測定した。焼結体から、全長３６閤以上１幅４
．０±０．１閣、厚さ３．０±０．１閣の角柱を研削し
、上下面の粗さをＪＩＳ Ｂ ０６０１に規定する０、
８Ｓ以下とし、これを試験片として、ＪＩＳ Ｒ−１６
０１に規定する。３点曲げ強さを測定した。Using this container in a nitrogen gas atmosphere (1 atm) at 1850℃
It was sintered under atmospheric pressure for 2 hours. The density of the obtained AYN sintered body was measured. From a sintered body, the total length is 36 or more, 1 width is 4
．． A square pillar with a thickness of 3.0 ± 0.1 mm and a thickness of 3.0 ± 0.1 mm is ground, and the roughness of the upper and lower surfaces is 0, as specified in JIS B 0601.
8S or less, and use this as a test piece, JIS R-16
01. Three-point bending strength was measured.
さらに、この焼結体の不純物酸素の分析を速中性子放射
化分析により行なった（東芝＠ＮＡＴ−ＺＯＯ−ＩＣ使
用）、上記焼結条件および得られた焼結体の特性を第１
表に示した。Furthermore, impurity oxygen in this sintered body was analyzed by fast neutron activation analysis (using Toshiba @NAT-ZOO-IC).The above sintering conditions and the characteristics of the obtained sintered body were
Shown in the table.
失適五ｌ二旦
焼結添加物の添加量を種々に変えて上記実施例１と同様
にしてＡｕＮ焼結体を製造し、それぞれについて、同様
に、評価を行なった。AuN sintered bodies were produced in the same manner as in Example 1 with various addition amounts of the second sintering additive, and each was evaluated in the same manner.
夾産五立ニヱ
焼結添加物の添加量および焼結温度を種々に変えて上記
実施例１と同様にしてＡ旦Ｎ焼結体を製造し、それぞれ
について同様に評価を行なった。AdanN sintered bodies were produced in the same manner as in Example 1 above by varying the amount of additives added and the sintering temperature, and each was evaluated in the same manner.
失五五ｌ二ｌ
焼結温度を種々に変えて上記実施例１と同様にしてＡｆ
ＬＮ焼結体を製造し、それぞれについて同様の評価を行
なった。Af
LN sintered bodies were manufactured and the same evaluations were performed on each of them.
失直旌胆
Ａ！１．Ｎ原料粉末の粒径、不純物酸素量および焼結温
度を変えて上記実施例１と同様にしてＡｆｉＮ焼結体を
製造し、同様の評価を行なった。Loss of directness A! 1. AfiN sintered bodies were produced in the same manner as in Example 1, except that the particle size of the N raw material powder, the amount of impurity oxygen, and the sintering temperature were changed, and the same evaluations were performed.
叉１舅旦二■
焼結添加物の添加量、焼結温度および焼結雰囲気および
雰囲気圧力を種々に変えて上記実施例１と同様にしてＡ
！；ＬＮ焼結体を製造し、それぞれについて同様の評価
を行なった。A was carried out in the same manner as in Example 1 by varying the amount of sintering additives, sintering temperature, sintering atmosphere, and atmospheric pressure.
! ;LN sintered bodies were manufactured and the same evaluation was performed on each of them.
来適五胆
焼結添加物の添加量、焼結温度および焼結時間を変えて
上記実施例１と同様にしてＡＬＮ焼結体を製造し、同様
の評価を行なった。ALN sintered bodies were produced in the same manner as in Example 1, except that the amount of the sintering additive added, the sintering temperature, and the sintering time were changed, and the same evaluation was performed.
寒直涯旦二且
焼結時間を種々に変えて上記実施例１と同様にしてＡｕ
Ｎ焼結体を製造し、それぞれについて同様の評価を行な
った。Au
N sintered bodies were manufactured and the same evaluations were performed on each.
１１涯丘
不純物としての酸素を３重量％含有し、平均粒径が１．
８−のＡｓＬＮ粉末に、添加物として平均粒径０．９−
のＹ２Ｏ２をイツトリウム元素の重量換算で２重量％添
加した。成形、脱脂までの行程および焼成用容器は上記
実施例と同様である。窒化ガス１０気圧の加圧中１８０
０℃、２時間で焼結した。得られた焼結体は上記実施例
１と同様に評価を行なった。11 Contains 3% by weight of oxygen as an impurity, and has an average particle size of 1.
8- AsLN powder with an average particle size of 0.9- as an additive.
Y2O2 was added in an amount of 2% by weight in terms of the weight of yttrium element. The steps from molding to degreasing and the firing container were the same as in the above example. 180 during pressurization of nitriding gas at 10 atmospheres
Sintering was carried out at 0°C for 2 hours. The obtained sintered body was evaluated in the same manner as in Example 1 above.
ス１１引１
焼結時間を変えた点を除き、上記実施例１７と同様にし
てＡ、ｄＮ焼結体を製造し、同様の評価を行なった。S11 1 A, dN sintered body was produced in the same manner as in Example 17 above, except that the sintering time was changed, and the same evaluation was performed.
失１０■旦
不純物としての酸素を０．５重量％含有し、平均粒径が
２．９．のＡｉＮ粉末に、添加物として平均粒径０．９
−のＹ２Ｏ，をイツトリウム元素の重量換算で４重量％
添加した。成形、脱脂までの行程および焼成用容器は上
記実施例１と同様である。窒化ガス減圧雰囲気中（０，
１気圧） １９００℃において２時間焼結し、同様の評
価を行なった。It contains 0.5% by weight of oxygen as an impurity and has an average particle size of 2.9. AiN powder with an average particle size of 0.9 as an additive.
- Y2O, 4% by weight in terms of the weight of yttrium element
Added. The steps from molding to degreasing and the firing container were the same as in Example 1 above. In a nitriding gas reduced pressure atmosphere (0,
1 atm)) Sintered at 1900° C. for 2 hours and evaluated in the same way.
失凰五刈二並
添加物の陽イオンを種々の希土類元素に変えて上記実施
例１と同様にしてＡ！；ＬＮ焼結体を製造し、それぞれ
について同様の評価を行なった。A! A! ;LN sintered bodies were manufactured and the same evaluation was performed on each of them.
１直舊互二堕
不純物としての酸素を０．４８重量％含有し、平均粒径
が２．９−のＡＬＮ粉末に、添加物として平均粒径０．
９−のＹＩＩ０２をイツトリウム元素の重量換算で４重
量％添加した。焼成用容器を種々に変えて。Additives to ALN powder containing 0.48% by weight of oxygen as an impurity and having an average particle size of 2.9% are added as additives.
9-YII02 was added in an amount of 4% by weight in terms of the weight of yttrium element. By changing the firing container.
上記実施例１と同様にしてＯＮ焼結体を製造し、それぞ
れについて同様の評価を行なった。ON sintered bodies were manufactured in the same manner as in Example 1 above, and the same evaluations were performed on each.
叉産五胆二用
不純物としての酸素を０．２６重量％含有し、平均粒径
が５．８ｐのＡｉＮ粉末に、添加物として平均粒径０．
９．のＹ、０．をイツトリウム元素の重量換算で２．５
重量％添加した。焼成用容器を種々に変えて、上記実施
例１と同様にしてｉＮ焼結体を製造しそれぞれについて
同様の評価を行なった。AiN powder containing 0.26% by weight of oxygen as an impurity and having an average particle size of 5.8p was added as an additive with an average particle size of 0.26% by weight.
9. Y, 0. is 2.5 in terms of weight of yttrium element.
% by weight was added. iN sintered bodies were produced in the same manner as in Example 1, using various firing containers, and the same evaluations were conducted for each.
失適五■二昇
不純物としての酸素を０．５９重量％含有し、平均粒径
が２．０−のＡｉＮ粉末に、添加物として平均粒径０．
９ｐのＹ２Ｏ，をイツトリウム元素の重量換算で２．５
重量％添加した。焼成用容器を種々に変えて、上記実施
例１と同様にしてＡＱＮ焼結体を製造し、それぞれにつ
いて同様の評価を行なった。An additive having an average particle size of 0.5% is added to the AiN powder containing 0.59% by weight of oxygen as an impurity and having an average particle size of 2.0.
9p of Y2O, converted to the weight of yttrium element, is 2.5
% by weight was added. AQN sintered bodies were produced in the same manner as in Example 1, using various firing containers, and the same evaluations were conducted for each.
崖較五エニュ
実施例１と同様な方法により得たＡユＮ脱脂体を、比較
例１では内側の全体がカーボン製の容器（焼結容器Ａ）
、比較例２では内側の全体がｉＮｇの容器、比較例３で
は内側の全体がタングステン製の容器を用い、１８５０
℃、２ｈｒ、Ｎ、気流中で常圧焼結し、焼結体を得た。In Comparative Example 1, a degreased body obtained by the same method as in Example 1 was placed in a container whose entire inside was made of carbon (sintered container A).
, Comparative Example 2 uses a container whose inside is entirely made of iNg, and Comparative Example 3 uses a container whose inside is entirely made of tungsten.
C. for 2 hours under atmospheric pressure in a N air stream to obtain a sintered body.
これらの焼結体の特性を表２表に示す、また、得られた
焼結体は、表面が粗で、変形していた。この結果より、
少なくとも、内部の一部がアルミナよりなる焼結容器を
用いない場合は、高強度を有する。表面状態の良好なｉ
Ｎ焼結体が得られず、アルミナ雰囲気の有効さがわかる
。The properties of these sintered bodies are shown in Table 2, and the surfaces of the obtained sintered bodies were rough and deformed. From this result,
At least when a sintered container whose interior is partially made of alumina is not used, it has high strength. i with good surface condition
No N sintered body was obtained, demonstrating the effectiveness of an alumina atmosphere.
（以下余白）
〔発明の効果ノ
以上述べた如く、本発明の窒化アルミニウム焼結体の製
造方法は、Ｊｌ密で焼き上がり状態の良好な、高強度を
有するという優れた窒化アルミニウム焼結体を提供する
ものであり、その工業的価値は極めて大きいものである
。(Left below) [Effects of the Invention] As described above, the method for producing an aluminum nitride sintered body of the present invention produces an excellent aluminum nitride sintered body that is Jl dense, has a good firing state, and has high strength. and its industrial value is extremely large.
代理人 弁理士 則 近 憲 佑 同 松山光之Agent: Patent Attorney Noriyuki Chika Same as Mitsuyuki Matsuyama
Claims (2)
径が０．０５〜１０μｍである窒化アルミニウム粉末と
、IIａ族、IIIａ族及びＣａ、ＳｒなどのIIａ族化合物
、Ｙ、ＬａなどのIIIａ族化合物および希土類元素を重
量換算で０．０１〜１５重量％の含有するIIａ族化合物
、IIIａ族化合物及び／又は希土類元素化合物とを混合
したのち成形した成形体を ｂ）Ａｌ＿２Ｏ＿３製容器中、もしくは、Ａｌ＿２Ｏ＿
３焼結体またはＡｌ＿２Ｏ＿３粉末で焼成中に（Ａｌ−
Ｏ）ガス雰囲気をつくり出す容器中で ｃ）非酸化性ガス雰囲気、１５５０〜２０５０℃の条件
で焼成することを特徴とした窒化アルミニウム焼結体の
製造方法。(1) a) Aluminum nitride powder with an impurity oxygen content of 5% by weight or less and an average particle size of 0.05 to 10 μm, and group IIa, group IIIa, and group IIa compounds such as Ca and Sr, Y, and La. b) A container made of Al_2O_3, which is formed by mixing a group IIIa compound such as a group IIIa compound and a rare earth element containing 0.01 to 15% by weight of a rare earth element, a group IIIa compound, and/or a rare earth element compound. Medium or Al_2O_
3 sintered body or Al_2O_3 powder during firing (Al-
O) A method for producing an aluminum nitride sintered body, characterized by firing in a container that creates a gas atmosphere, c) in a non-oxidizing gas atmosphere, at a temperature of 1550 to 2050°C.
＾２以上である特許請求の範囲第１項記載の窒化アルミ
ニウム焼結体の製造方法。(2) Relative density 85% or more, bending strength 20kgcm^-
The method for producing an aluminum nitride sintered body according to claim 1, wherein the aluminum nitride sintered body is ^2 or more.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62110809A JPS63277572A (en) | 1987-05-08 | 1987-05-08 | Production of sintered aluminum nitride |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62110809A JPS63277572A (en) | 1987-05-08 | 1987-05-08 | Production of sintered aluminum nitride |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS63277572A true JPS63277572A (en) | 1988-11-15 |
Family
ID=14545207
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62110809A Pending JPS63277572A (en) | 1987-05-08 | 1987-05-08 | Production of sintered aluminum nitride |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS63277572A (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH03126673A (en) * | 1989-10-12 | 1991-05-29 | Fujitsu Ltd | Production of sintered aluminum nitride |
| JP2008074643A (en) * | 2006-09-19 | 2008-04-03 | Tokuyama Corp | Method for burning aluminum nitride |
| JP2012036090A (en) * | 2011-10-26 | 2012-02-23 | Tokuyama Corp | Method for producing aluminum nitride sintered compact |
-
1987
- 1987-05-08 JP JP62110809A patent/JPS63277572A/en active Pending
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH03126673A (en) * | 1989-10-12 | 1991-05-29 | Fujitsu Ltd | Production of sintered aluminum nitride |
| JP2008074643A (en) * | 2006-09-19 | 2008-04-03 | Tokuyama Corp | Method for burning aluminum nitride |
| JP2012036090A (en) * | 2011-10-26 | 2012-02-23 | Tokuyama Corp | Method for producing aluminum nitride sintered compact |
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