JPH0365563A - Production of aluminum nitride sintered compact - Google Patents
Production of aluminum nitride sintered compactInfo
- Publication number
- JPH0365563A JPH0365563A JP1201819A JP20181989A JPH0365563A JP H0365563 A JPH0365563 A JP H0365563A JP 1201819 A JP1201819 A JP 1201819A JP 20181989 A JP20181989 A JP 20181989A JP H0365563 A JPH0365563 A JP H0365563A
- Authority
- JP
- Japan
- Prior art keywords
- aluminum
- containing compound
- urea
- aluminum nitride
- mixture
- 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 31
- 238000004519 manufacturing process Methods 0.000 title claims description 16
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 40
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 36
- 150000001875 compounds Chemical class 0.000 claims abstract description 28
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims abstract description 21
- 239000004202 carbamide Substances 0.000 claims abstract description 21
- 239000007864 aqueous solution Substances 0.000 claims abstract description 19
- 239000000203 mixture Substances 0.000 claims abstract description 18
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000012298 atmosphere Substances 0.000 claims abstract description 9
- 238000002156 mixing Methods 0.000 claims abstract description 9
- -1 aluminum alkoxide Chemical class 0.000 claims abstract description 7
- 238000005245 sintering Methods 0.000 claims abstract description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 5
- 230000001590 oxidative effect Effects 0.000 claims abstract description 5
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical compound Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 abstract description 16
- BNGXYYYYKUGPPF-UHFFFAOYSA-M (3-methylphenyl)methyl-triphenylphosphanium;chloride Chemical compound [Cl-].CC1=CC=CC(C[P+](C=2C=CC=CC=2)(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 BNGXYYYYKUGPPF-UHFFFAOYSA-M 0.000 abstract description 3
- DIZPMCHEQGEION-UHFFFAOYSA-H aluminium sulfate (anhydrous) Chemical compound [Al+3].[Al+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O DIZPMCHEQGEION-UHFFFAOYSA-H 0.000 abstract description 2
- 229910052761 rare earth metal Inorganic materials 0.000 abstract description 2
- 150000003839 salts Chemical class 0.000 abstract description 2
- 229910052784 alkaline earth metal Inorganic materials 0.000 abstract 1
- 150000001342 alkaline earth metals Chemical class 0.000 abstract 1
- 238000000034 method Methods 0.000 description 11
- 238000001035 drying Methods 0.000 description 9
- 239000000843 powder Substances 0.000 description 8
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 6
- 229910052799 carbon Inorganic materials 0.000 description 6
- 239000012299 nitrogen atmosphere Substances 0.000 description 6
- 238000000465 moulding Methods 0.000 description 5
- 239000000758 substrate Substances 0.000 description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 238000003869 coulometry Methods 0.000 description 4
- 238000010304 firing Methods 0.000 description 4
- 230000009467 reduction Effects 0.000 description 4
- 239000011343 solid material Substances 0.000 description 4
- VXYADVIJALMOEQ-UHFFFAOYSA-K tris(lactato)aluminium Chemical compound CC(O)C(=O)O[Al](OC(=O)C(C)O)OC(=O)C(C)O VXYADVIJALMOEQ-UHFFFAOYSA-K 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- 229910002651 NO3 Inorganic materials 0.000 description 3
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 3
- 238000005121 nitriding Methods 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- 101100397221 Rhodococcus sp. (strain AD45) isoI gene Proteins 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 239000004411 aluminium Substances 0.000 description 2
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- VKYKSIONXSXAKP-UHFFFAOYSA-N hexamethylenetetramine Chemical compound C1N(C2)CN3CN1CN2C3 VKYKSIONXSXAKP-UHFFFAOYSA-N 0.000 description 2
- JVTAAEKCZFNVCJ-UHFFFAOYSA-N lactic acid Chemical compound CC(O)C(O)=O JVTAAEKCZFNVCJ-UHFFFAOYSA-N 0.000 description 2
- OQUOOEBLAKQCOP-UHFFFAOYSA-N nitric acid;hexahydrate Chemical compound O.O.O.O.O.O.O[N+]([O-])=O OQUOOEBLAKQCOP-UHFFFAOYSA-N 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- WGTYBPLFGIVFAS-UHFFFAOYSA-M tetramethylammonium hydroxide Chemical compound [OH-].C[N+](C)(C)C WGTYBPLFGIVFAS-UHFFFAOYSA-M 0.000 description 2
- QBAZWXKSCUESGU-UHFFFAOYSA-N yttrium(3+);trinitrate;hexahydrate Chemical compound O.O.O.O.O.O.[Y+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O QBAZWXKSCUESGU-UHFFFAOYSA-N 0.000 description 2
- 229910000838 Al alloy Inorganic materials 0.000 description 1
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 description 1
- 241001313637 Isotria Species 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 1
- JPUHCPXFQIXLMW-UHFFFAOYSA-N aluminium triethoxide Chemical compound CCO[Al](OCC)OCC JPUHCPXFQIXLMW-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000001110 calcium chloride Substances 0.000 description 1
- 229910001628 calcium chloride Inorganic materials 0.000 description 1
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 description 1
- 239000000292 calcium oxide Substances 0.000 description 1
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000010292 electrical insulation Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000004312 hexamethylene tetramine Substances 0.000 description 1
- 235000010299 hexamethylene tetramine Nutrition 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000011810 insulating material Substances 0.000 description 1
- 239000004310 lactic acid Substances 0.000 description 1
- 235000014655 lactic acid Nutrition 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- MAJZZCVHPGUSPM-UHFFFAOYSA-N nitric acid nonahydrate Chemical compound O.O.O.O.O.O.O.O.O.O[N+]([O-])=O MAJZZCVHPGUSPM-UHFFFAOYSA-N 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- WEQHQGJDZLDFID-UHFFFAOYSA-J thorium(iv) chloride Chemical compound Cl[Th](Cl)(Cl)Cl WEQHQGJDZLDFID-UHFFFAOYSA-J 0.000 description 1
- WOZZOSDBXABUFO-UHFFFAOYSA-N tri(butan-2-yloxy)alumane Chemical compound [Al+3].CCC(C)[O-].CCC(C)[O-].CCC(C)[O-] WOZZOSDBXABUFO-UHFFFAOYSA-N 0.000 description 1
- UAEJRRZPRZCUBE-UHFFFAOYSA-N trimethoxyalumane Chemical compound [Al+3].[O-]C.[O-]C.[O-]C UAEJRRZPRZCUBE-UHFFFAOYSA-N 0.000 description 1
- OBROYCQXICMORW-UHFFFAOYSA-N tripropoxyalumane Chemical compound [Al+3].CCC[O-].CCC[O-].CCC[O-] OBROYCQXICMORW-UHFFFAOYSA-N 0.000 description 1
Landscapes
- Ceramic Products (AREA)
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
この発明は、例えば、高熱伝導性（絶縁）基板として用
いるのに通した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 [Industrial Field of Application] The present invention relates to a method for producing a sintered aluminum nitride body for use, for example, as a highly thermally conductive (insulating) substrate.
ｉｃ等に代表される半導体素子の高集積化や大電力化が
進み、これに伴って、放熱性の良い電気絶縁材料が要求
されるようになった。これに応えて各種の高熱伝導性基
板が提案されている。その中でも、特に窒化アルミニウ
ムセラミソク基板が、熱伝導性、熱膨張性、電気絶縁性
等の点で優れていることから、実用化が進められてきて
いる。BACKGROUND ART As semiconductor devices such as ICs have become more highly integrated and have higher power, electrical insulating materials with good heat dissipation properties have become required. In response to this demand, various highly thermally conductive substrates have been proposed. Among these, aluminum nitride ceramic substrates in particular are being put into practical use because they are excellent in terms of thermal conductivity, thermal expansion, electrical insulation, and the like.
この窒化アルミニウムセラミック基板ば、アルミニウム
粉末を用いて得た焼結体である。しかしながら、従来、
十分な性能の窒化アルミニウム焼結体がなかなか得られ
なかったり、高価であったりという不具合があった。こ
こで用いられる窒化アルミニウム粉末は、アルミニウム
の直接窒化やアルミナの炭素還元等によって製造されて
いるが、例えば、アルミニウムの直接窄化法においては
、高純度で粒径の小さな粉末を得ることが困難であり、
アルミナの炭素還元法においては、反応に高温を要する
、原料価格が高い等の問題があるのである。アルミナの
炭素還元法の改良として、アル主ニウム源を炭素含有化
合物で還元する方法が提案されているが、還元効率の点
で、まだ十分とは言えない。This aluminum nitride ceramic substrate is a sintered body obtained using aluminum powder. However, conventionally,
There were problems in that aluminum nitride sintered bodies with sufficient performance were difficult to obtain and were expensive. The aluminum nitride powder used here is manufactured by direct nitriding of aluminum, carbon reduction of alumina, etc. However, for example, it is difficult to obtain powder with high purity and small particle size using the direct thinning method of aluminum. and
The carbon reduction method for alumina has problems such as high temperatures required for the reaction and high raw material costs. As an improvement to the carbon reduction method for alumina, a method has been proposed in which the main source of aluminum is reduced with a carbon-containing compound, but this method is still not sufficient in terms of reduction efficiency.
それに、−旦、窒化アルミニウム粉末を得る従来のプロ
セスは、手間がかかり、材料費やエネルギー費も結構高
くつくものであるため、結果的に製造される窒化アルミ
ニウム焼結体が高価なものになっている。In addition, the conventional process for obtaining aluminum nitride powder is labor-intensive and requires considerable material and energy costs, making the resulting aluminum nitride sintered body expensive. ing.
この発明は、このような事情に鑑み、十分に焼結された
緻密な窒化アルミニウム焼結体を簡単かつ安価に得るこ
とのできる方法を提供することを課題とする。In view of these circumstances, it is an object of the present invention to provide a method that can easily and inexpensively obtain a sufficiently sintered and dense aluminum nitride sintered body.
〔課題を解決するための手段〕
前記課題を解決するため、請求項１記載の窒化アルミニ
ウム焼結体の製造方法では、アルミニウム含有化合物と
尿素の混合物からなる所定形状の成形体を、窒素を含む
非酸化性雰囲気下で焼成するようにしている。[Means for Solving the Problems] In order to solve the above problems, in the method for producing an aluminum nitride sintered body according to claim 1, a molded body of a predetermined shape made of a mixture of an aluminum-containing compound and urea is made of a mixture containing nitrogen. The firing is done in a non-oxidizing atmosphere.
この発明の製造方法で用いられるアルミニウム含有化合
物と尿素の混合物としては、例えば、請求項２記載の発
明のように、アルミニウム含有化合物が水溶性化合物で
あり、これと尿素を水溶液状態で均一に混合させた後、
水分を除くことにより得たものが挙げられる。In the mixture of an aluminum-containing compound and urea used in the production method of the present invention, for example, as in the invention according to claim 2, the aluminum-containing compound is a water-soluble compound, and the aluminum-containing compound and urea are uniformly mixed in an aqueous solution state. After letting
Examples include those obtained by removing water.
この発明の製造方法に用いられるアルミニウム含有化合
物としては、請求項３記載の発明のように、アルくニウ
ム多核錯体およびアルミニウムアルコキシドのうちの少
なくともひとつが挙げられる。The aluminum-containing compound used in the production method of the present invention includes at least one of an aluminium polynuclear complex and an aluminum alkoxide, as in the third aspect of the invention.
この発明にかかる窒化アルミニウム焼結体の製造方法で
は、例えば、請求項４記載の発明のように、成形体に焼
結助剤を含ませて焼成するようにしてもよい。In the method for producing an aluminum nitride sintered body according to the present invention, for example, as in the fourth aspect of the present invention, the molded body may contain a sintering aid and then be fired.
以下、より具体的に説明する。This will be explained in more detail below.
アルくニウム含有化合物は、窒化アルミニウムの主体で
あるアルミニウムの供給源となるものである。したがっ
て、アルミニウムを含む化合物であれば、特に限定され
ることはないが、例えば、硝酸アル主ニウム、塩化アル
ミニウム、硫酸アルミニウム、水酸化アルミニウム、乳
酸アル主ニウム、アルミナ、アルミニウム多核錯体、ア
ルミニウムアルコキシド等がある。The aluminium-containing compound is a source of aluminum, which is the main component of aluminum nitride. Therefore, as long as it is a compound containing aluminum, it is not particularly limited, but examples include aluminum nitrate, aluminum chloride, aluminum sulfate, aluminum hydroxide, aluminum lactate, alumina, aluminum polynuclear complex, aluminum alkoxide, etc. There is.
アルミニウム多核錯体としては、塩基性塩化アルミニウ
ム、塩基性乳酸アルミニウム、塩基性硝酸アルくニウム
等が例示される。Examples of the aluminum polynuclear complex include basic aluminum chloride, basic aluminum lactate, and basic aluminum nitrate.
アルミニウムアルコキシド（アルミニウムアルコキサイ
ド）としては、アルミニウムメトキシド、アルミニウム
エトキシド、アルミニウムプロポキシド、アルミニウム
ブトキシド等の炭素数１０以下の脂肪族のアルコキシド
が好適に使用できるなお、前記のアルミニウム含有化合
物は、単独で、あるいは、複数種併用して用いる。As the aluminum alkoxide, aliphatic alkoxides having 10 or less carbon atoms such as aluminum methoxide, aluminum ethoxide, aluminum propoxide, and aluminum butoxide can be suitably used. Used alone or in combination.
尿素は、焼成工程での窒化アルミニウムの生成反応にお
いて、前記アルミニウム含有化合物中に含まれる酸素元
素を、ＣＯ，ＣＯｘ０形で除去する作用を果たす。Urea functions to remove the oxygen element contained in the aluminum-containing compound in the form of CO and COx0 in the aluminum nitride production reaction in the firing process.
アルミニウム含有化合物が水溶性化合物であり、これと
尿素を水溶液状態で均一に混合させた後、乾燥させて水
分を除くことにより混合物を得る場合、乾燥温度は、例
えば７０〜２００℃程度の範囲が適当である。When the aluminum-containing compound is a water-soluble compound and a mixture is obtained by uniformly mixing this and urea in an aqueous solution state and then drying to remove water, the drying temperature is, for example, in the range of about 70 to 200°C. Appropriate.
このように乾燥して得られた混合物は、粉末状態、ある
いは、バルク状態である。この発明の製造方法では、混
合物を所定形状の成形体とするわけであるが、乾燥して
得られる混合物がバルク状であった場合、−旦、粉砕し
粉末化してから成形することが好ましいが、バルク状の
まま成形するようにしてもよい。The mixture obtained by drying in this way is in a powder state or a bulk state. In the manufacturing method of the present invention, the mixture is formed into a molded body of a predetermined shape, but if the mixture obtained by drying is in bulk form, it is preferable to first crush and powder it and then mold it. , it may also be molded in bulk form.
成形方法は、例えば、成形金型を用いた加圧成形法など
が用いられるが、不都合な成分の変質や流密を招来しな
い方法であればよく、特に限定されない。The molding method may be, for example, a pressure molding method using a mold, but is not particularly limited as long as it does not cause undesirable deterioration or leakage of components.
成形体に含まれる焼結助剤としては、アルカリ土類、あ
るいは、希土類元素の塩や酸化物等が挙げられる。例え
ば、硝酸イソトリウム、塩化７ｆ／トリウム１、塩基性
酢酸イソＩ・り省″ノム、酸化７ｆ、、ｌ、リウｌへ、
硝酸カルシラ五、塩化カルシ１′）ム、酸化カルシ・：
ノム等が具体的ｔ、′４例示７′（れるが１、これに駆
足されない。なお、焼結助剤の含有量は含をアルミニウ
ムに対して３−＝１０重景重電度が好４何９．い焼結助
剤を添加するタイミ゛／グは、アルミて、すＪい含有化
合物と尿素か混合され人・水溶液段階、あるいは、水溶
液乾繰後の粉末段階・専いＶれであ−。Examples of the sintering aid contained in the compact include salts and oxides of alkaline earth or rare earth elements. For example, isotrium nitrate, 7f/thorium chloride, basic acetic acid isoI, 7f, 1, liu,
Calcium nitrate, Calcium chloride, Calcium oxide:
Nome etc. are specific, '4 example 7' (1, but this is not sufficient.The content of the sintering aid is preferably 3-=10 heavy density for aluminum. 4/9. The timing to add the sintering aid is when the aluminum alloy is mixed with the urea-containing compound at the aqueous solution stage, or at the powder stage after the aqueous solution has been dried. So...
てもよく、特に限定されない。may be used, and is not particularly limited.
非酸化性雰囲気と１，５．ては、窄素を含むアルボ１／
、窒素を含む−・醸化炭素、あるい＆Ｊ：、窒素、アン
モニア等の雰囲気が用いられる。焼成温庶は、１２００
℃以上、好ましくは、１４００へ−２００Ｏ℃程度であ
る。なお、窒化後、例ヌば、６００ ＝７００℃程度の
酸化性雰囲気で、＼らに加熱処理ｊ７焼結体内の残留炭
素を除＜ 、Ｊ、うにｊ２てもよい。Non-oxidizing atmosphere and 1,5. In this case, Arbo 1/
An atmosphere containing nitrogen, fermented carbon, nitrogen, ammonia, or the like is used. Firing temperature is 1200
℃ or higher, preferably about 1400 to 200°C. After nitriding, residual carbon in the sintered body may be removed by heat treatment, for example, in an oxidizing atmosphere at about 600° C. to 700° C.
この発明にかかる窒化アル宝ニウム焼結体の製ｊ告方ｔ
ｉ、：のよ・うに、ｊ′ルミ−“、ラム含有化合物、例
えば、アル失ニウム多核錯体やアルミーニーウムアルコ
ヤ・ンＶと尿素の混合物からなる所定形状の成形棒ろ二
１、窄素を含む非酸化性雰囲気下で焼成４″ると、純度
（窒化率）が高く緻密で熱伝導率のよい窒化アルミニウ
ム焼結体が、煩雑な粉末工程を経ることなく容易に得ら
れる、゛、ととなる。Manufacturing method of aluminum nitride sintered body according to this invention
i,: Like, j'lumi-'', a molded rod 1 of a predetermined shape made of a rum-containing compound, such as an alkali polynuclear complex or a mixture of aluminum alkoyane V and urea. By sintering in a non-oxidizing atmosphere containing elements, an aluminum nitride sintered body with high purity (nitridation rate), density, and good thermal conductivity can be easily obtained without going through a complicated powder process. , and so on.
尿素は窒素含イｆ化合物であるために混合物中と・こも
穿索源ををするので、局所的還元雰囲気が形成＝Ｕｘれ
混合物内部から窒化反応が促進され窒化アルミニウムが
迅速に形成される。Since urea is a nitrogen-containing compound, it also acts as a source of permeation in the mixture, so a local reducing atmosphere is formed and the nitriding reaction is promoted from within the mixture, resulting in the rapid formation of aluminum nitride.
１′ルミニウム含有化合物が水溶性化合物であり１、．
れと尿素を水溶液状態で均一に混合させた後５、水分を
除く、＝とにより得た混合物は、アルミニウム含有化合
物と尿素が分子オーダで混じり合った状態となるため１
．１：、り純度が高く均質な焼結体が得られるようにな
る。1' The aluminum-containing compound is a water-soluble compound and 1,.
After homogeneously mixing this and urea in an aqueous solution state, the mixture obtained by removing water is 1, since the aluminum-containing compound and urea are mixed on a molecular order.
．． 1: A homogeneous sintered body with high purity can be obtained.
以−′１・、具体的な実施例について説明する。 Hereinafter, specific examples will be described.
実施例１−
塩基性塩化アルミニウム含有量部に対し、尿素が４．０
重電部となるよ°うに混合した水溶液を作製した。なお
、塩基性塩化アルミニウムは、アルミニウム含有量がＡ
ｄオＯ７換算で５０電量％であり、塩基度が８４％のも
のを用いた。つぎム、二、この水溶液を７０℃の乾燥湿
度で蒸発乾固させた。Example 1 - Urea is 4.0 parts basic aluminum chloride content
An aqueous solution was prepared by mixing the two to form a heavy electric part. In addition, basic aluminum chloride has an aluminum content of A
The amount of electricity used was 50% in terms of dOO7, and the basicity was 84%. Next, this aqueous solution was evaporated to dryness at a dry humidity of 70°C.
得られた固形物を１、−目１、粉砕した後、成形金型を
用いて、直径２５Ｂ、厚み３ ｍｍの円板状の成形棒に
１７でから、１９００℃の窒素雰囲気で８時間焼成１，
１、窒化′アルくニウム焼結体を得た。After crushing the obtained solid material 1-1 times, it was molded into a disk-shaped rod with a diameter of 25 B and a thickness of 3 mm using a molding die, and then baked in a nitrogen atmosphere at 1900°C for 8 hours. 1,
1. A sintered body of aluminum nitride was obtained.
実施例２
実施例１で用いた塩基性塩化アルミニ、ラム１電置部に
対し、尿素が４６０電量部、硝酸イソトリウム６永和物
が０．０６８電量部となるように混合した水溶液を作Ｍ
ｌ、ｌこ。つぎに、この水溶液を８０℃の乾燥温度で蒸
発乾固さ−ｉｑた。得られた固形物を、−旦、粉砕Ｌ７
た後、成形金型を用いて、直径２５１１Ｉｍ、厚み３關
の円板状の成形棒にしてから、１８５０℃の窒素雰囲気
で４時間焼６成１７、窒化アルミニウム焼結体を（りた
。Example 2 An aqueous solution was prepared by mixing the basic aluminum chloride used in Example 1, 460 coulometric parts of urea, and 0.068 coulometric parts of isotrium nitrate 6 per 1 part of ram.
l-l-ko. Next, this aqueous solution was evaporated to dryness at a drying temperature of 80°C. The obtained solid was crushed L7
After that, using a molding die, it was formed into a disk-shaped rod with a diameter of 2511 Im and a thickness of 3 mm, and then fired in a nitrogen atmosphere at 1850° C. for 4 hours to form an aluminum nitride sintered body.
実施例３
塩基性乳酸アルミニウム１電量部に対し、尿素が３．６
徂ｉ１部、硝酸イソＩ・リウム６水和物が０．０５電
量部となるよ・うに混合した水溶液を作製した。なお、
塩基性乳酸アルミニウムは、アルミニウム含有量がＡＩ
！ｔｏ＊換算で３７銀量％であり７、乳酸含量５６％の
ものを用いた。つぎに、この水溶液を８０℃の乾燥温度
で蒸発乾固させた。得られた固形物を、−１１、粉砕し
た後、成形金型を用いて、直径２５州、厚み３翔のＰ］
根板状成形棒にしてから、１８５０℃の窒素雰囲気で４
時間焼成ｊ２、窒化アルミニ、リム焼結体を得た。Example 3 3.6 parts of urea per 1 coulometric part of basic aluminum lactate
An aqueous solution was prepared by mixing 1 part of nitrate and 0.05 part of coulometric amount of isoI.lium nitrate hexahydrate. In addition,
Basic aluminum lactate has an aluminum content of AI
! The silver content was 37% in terms of to*7, and the lactic acid content was 56%. Next, this aqueous solution was evaporated to dryness at a drying temperature of 80°C. After crushing the obtained solid material, using a mold, it was made into a P with a diameter of 25 mm and a thickness of 3 mm.
After forming a root plate-shaped rod, it was heated in a nitrogen atmosphere at 1850℃ for 4 hours.
A time-fired j2, aluminum nitride, rim sintered body was obtained.
実施例４
アルミ′−１リムトリイソプロポキシド（アルミニ１″
）人トリイソブ１コ２１ミキサイド）１重量部、尿素３
゜８重間部、硝酸イソトリウム６水和物０．０３３１ｉ
量部を、テトラメチルアンモニウムハイドロオキ４り・
イ１′１５％水溶液２．９７重量部に加え、室温で１時
間かく拌した後、この溶液を８０℃の乾燥温度で蒸′９
．乾固、＼−１工た。得られた固形物を粉砕した後、実
施例１と同様に成形体を得た後、１８５０℃の温度下、
窒素雰囲気で４時間焼成し、窒化アルミニウム焼結体を
得た。Example 4 Aluminum'-1 rim triisopropoxide (aluminum 1"
) 1 part by weight of human triisobut 21 mixture), 3 parts by weight of urea
゜octium, isotria nitrate hexahydrate 0.0331i
4 parts of tetramethylammonium hydroxide
B1' Add to 2.97 parts by weight of a 15% aqueous solution, stir at room temperature for 1 hour, and then evaporate this solution at a drying temperature of 80°C.
．． Dry, ＼-1 k. After pulverizing the obtained solid material and obtaining a molded body in the same manner as in Example 1, at a temperature of 1850°C,
The aluminum nitride sintered body was obtained by firing in a nitrogen atmosphere for 4 hours.
一実施例５−
硝酸アルくニウム９水和物１重量部に対し、尿素が４．
０重量部、硝酸イツトリウム６水和物が０゜０１９重量
部となるように混合した水溶液を作製した。つぎに、こ
の水溶液を１２０℃の乾燥温度で蒸発乾固させた。得ら
れた固形物を粉砕してから実施例１と同様にして成形体
を得た後、１８５０℃の温度下、窒素雰囲気で４時間焼
成し、窒化アルミニウム焼結体を得た。Example 5 - 4.0 parts of urea was added to 1 part by weight of alkium nitrate nonahydrate.
An aqueous solution was prepared by mixing 0 parts by weight of yttrium nitrate hexahydrate and 0.019 parts by weight of yttrium nitrate hexahydrate. Next, this aqueous solution was evaporated to dryness at a drying temperature of 120°C. The obtained solid was pulverized and a molded body was obtained in the same manner as in Example 1, and then fired at a temperature of 1850° C. in a nitrogen atmosphere for 4 hours to obtain an aluminum nitride sintered body.
一比較例１−０
塩基性塩化アルミニウム１重量部に対し、ヘキサメチレ
ンテトラミンが０．４７重量部となるように混合した水
溶液を作製した。なお、塩基性塩化アルミニウムは、ア
ルミニウム含有量がＡｌｔ。Comparative Example 1-0 An aqueous solution was prepared by mixing 1 part by weight of basic aluminum chloride with 0.47 parts by weight of hexamethylenetetramine. Note that basic aluminum chloride has an aluminum content of Alt.
、換算で５０重量％であり、塩基度が８４％のものを用
いた。つぎに、この水溶液を１２０℃の乾燥温度で蒸発
乾固させた。得られた固形物を、−旦、粉砕した後、成
形金型を用いて、直径２５ｆｌ、厚み３１１の円板状の
成形体にしてから、１９００℃の窒素雰囲気で８時間焼
成し、窒化アルミニウム焼結体を得た。, and the basicity was 84%. Next, this aqueous solution was evaporated to dryness at a drying temperature of 120°C. The obtained solid material was first pulverized, and then made into a disc-shaped molded product with a diameter of 25 fl and a thickness of 311 cm using a molding die, and then fired in a nitrogen atmosphere at 1900°C for 8 hours to form aluminum nitride. A sintered body was obtained.
このようにして得られた実施例１〜５および比較例１の
窒化アルミニウム焼結体の密度と熱伝導率を測定した。The density and thermal conductivity of the aluminum nitride sintered bodies of Examples 1 to 5 and Comparative Example 1 thus obtained were measured.
測定結果を第１表に記す。The measurement results are shown in Table 1.
第 １ 表
実施例１〜５の窒化アル主ニウム焼結体は、第１表にみ
るように、比較例１のそれに比べて、大きな密度をもつ
緻密な焼結体であり、しかも、純度が高く高熱伝導率で
ある。実施例１〜５の焼結体をＸ線分析したところ、未
窒化の残留Ａ７２．０８の存在を示すピークは殆ど検出
されなかったが、比較例１の焼結体をＸ線分析したとこ
ろ、未窒化の残留Ａ ｌ ｘ Ｏｔの存在を示すピーク
が明瞭に検出された。Table 1 As shown in Table 1, the aluminum nitride-based sintered bodies of Examples 1 to 5 are dense sintered bodies with higher densities than those of Comparative Example 1, and have a higher purity. High thermal conductivity. When the sintered bodies of Examples 1 to 5 were subjected to X-ray analysis, almost no peak indicating the presence of unnitrided residual A72.08 was detected, but when the sintered bodies of Comparative Example 1 were subjected to X-ray analysis, A peak indicating the presence of unnitrided residual Al x Ot was clearly detected.
以上に述べたように、この発明にかかる窒化アルミニウ
ム焼結体の製造方法では、窒化アルミニウム粉末の状態
を経ることなく、緻密で高熱伝導性の焼結体を直に製造
できる。そのため、優れた高熱伝導性（絶縁）基板が安
価かつ容易に得られるようになる。As described above, in the method for producing an aluminum nitride sintered body according to the present invention, a dense and highly thermally conductive sintered body can be directly produced without going through the state of aluminum nitride powder. Therefore, an excellent high thermal conductivity (insulating) substrate can be obtained easily and inexpensively.
また、この製造方法において、混合物が、アルミニウム
含有化合物と尿素を水溶液状態で均一に混合させた後、
水分を除くようにして得たものであると、アルミニウム
含有化合物と尿素が十分に混ｊニり合うようになるため
、より高純度で均質／Ｉ（焼結体が得られるようになる
。In addition, in this manufacturing method, after the mixture is uniformly mixed with an aluminum-containing compound and urea in an aqueous solution state,
If the product is obtained by removing moisture, the aluminum-containing compound and urea will be sufficiently mixed, so that a homogeneous sintered body with higher purity can be obtained.
Claims (1)
定形状の成形体を、窒素を含む非酸化性雰囲気下で焼成
するようにする窒化アルミニウム焼結体の製造方法。 ２ アルミニウム含有化合物が水溶性化合物であり、こ
れと尿素を水溶液状態で均一に混合させた後、水分を除
くことにより混合物を得る請求項１記載の窒化アルミニ
ウム焼結体の製造方法。 ３ アルミニウム含有化合物が、アルミニウム多核錯体
およびアルミニウムアルコキシドのうちの少なくともひ
とつである請求項１または２記載の窒化アルミニウム焼
結体の製造方法。 ４ 成形体に焼結助剤が含まれてなる請求項１から３ま
でのいずれかに記載の窒化アルミニウム焼結体の製造方
法。[Scope of Claims] 1. A method for producing an aluminum nitride sintered body, in which a molded body of a predetermined shape made of a mixture of an aluminum-containing compound and urea is fired in a non-oxidizing atmosphere containing nitrogen. 2. The method for producing an aluminum nitride sintered body according to claim 1, wherein the aluminum-containing compound is a water-soluble compound, and the mixture is obtained by uniformly mixing this and urea in an aqueous solution state and then removing water. 3. The method for producing an aluminum nitride sintered body according to claim 1 or 2, wherein the aluminum-containing compound is at least one of an aluminum polynuclear complex and an aluminum alkoxide. 4. The method for producing an aluminum nitride sintered body according to any one of claims 1 to 3, wherein the molded body contains a sintering aid.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1201819A JPH0365563A (en) | 1989-08-02 | 1989-08-02 | Production of aluminum nitride sintered compact |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1201819A JPH0365563A (en) | 1989-08-02 | 1989-08-02 | Production of aluminum nitride sintered compact |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH0365563A true JPH0365563A (en) | 1991-03-20 |
Family
ID=16447431
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP1201819A Pending JPH0365563A (en) | 1989-08-02 | 1989-08-02 | Production of aluminum nitride sintered compact |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0365563A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103320899A (en) * | 2013-07-01 | 2013-09-25 | 中国计量学院 | Preparation method of nanometer aluminum nitride fiber |
-
1989
- 1989-08-02 JP JP1201819A patent/JPH0365563A/en active Pending
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103320899A (en) * | 2013-07-01 | 2013-09-25 | 中国计量学院 | Preparation method of nanometer aluminum nitride fiber |
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