JPS62283805A - Production of extremely fine aluminum nitride powder - Google Patents

Production of extremely fine aluminum nitride powder

Info

Publication number
JPS62283805A
JPS62283805A JP12466686A JP12466686A JPS62283805A JP S62283805 A JPS62283805 A JP S62283805A JP 12466686 A JP12466686 A JP 12466686A JP 12466686 A JP12466686 A JP 12466686A JP S62283805 A JPS62283805 A JP S62283805A
Authority
JP
Japan
Prior art keywords
nitrogen
atmosphere
powder
ammonia
aluminum nitride
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
JP12466686A
Other languages
Japanese (ja)
Other versions
JPH0460046B2 (en
Inventor
Masahiro Uda
雅広 宇田
Satoru Ono
悟 大野
Hideo Okuyama
秀男 奥山
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
National Research Institute for Metals
Original Assignee
National Research Institute for Metals
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by National Research Institute for Metals filed Critical National Research Institute for Metals
Priority to JP12466686A priority Critical patent/JPS62283805A/en
Publication of JPS62283805A publication Critical patent/JPS62283805A/en
Publication of JPH0460046B2 publication Critical patent/JPH0460046B2/ja
Granted legal-status Critical Current

Links

Classifications

    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J12/00Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor
    • B01J12/002Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor carried out in the plasma state

Abstract

PURPOSE:To produce the title extremely fine powder of AlN by using a gaseous mixture of N2 and NH3 or the gaseous mixture further added with an inert gas as the ambient atmosphere when metallic Al is melted in the frame of arc or a plasma jet to produce the fine powder. CONSTITUTION:Al 4 is charged in the heating furnace 5 in a closed vessel 8, and the inside of the closed vessel 8 is evacuated. The Al 4 is heated and melted in the heating furnace 5, gaseous N2 is introduced from a gas inlet 1 for a discharge electrode, and gaseous NH3 is introduced from an inlet 2 for an atmospheric gas as a spiral-flow gas around an arc plasma 3. In this case, the ratio of N2 to NH3 is controlled to 0.01-50, and the gaseous mixture is diluted, as required, with an inert gas to form a dilute (N2+NH3) gas atmosphere. The active chemical species such as NH2, NH, N, etc., formed by the decomposition of NH3 in the arc plasma 3 reacts with Al vapor, and extremely fine AlN powder is formed.

Description

【発明の詳細な説明】 3、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超微粉の製造法に関する。[Detailed description of the invention] 3. Detailed description of the invention Industrial applications The present invention relates to a method for producing ultrafine aluminum nitride powder.

窒化アルミニウム焼結体は、耐熱、高熱伝導、高絶縁性
などの特性を有することから、各種の半導体用放熱基板
、透光性耐熱材、弾性表面波素子基板、溶融金属用耐熱
浴材など広範な用途を有している。この窒化アルミニウ
ム焼結体は、一般に窒化アルミニウム粉末を焼結するこ
とにより製造されるが、得られる焼結体の特性は原料粉
末の純度、粒径に大きく影響を受け、高性能な窒化アル
ミニウム焼結体を得るためには、高純度で、かつ微細な
窒化アルミニウム粉を使用することが要求される。
Aluminum nitride sintered bodies have properties such as heat resistance, high thermal conductivity, and high insulation properties, so they are used in a wide range of applications such as heat dissipating substrates for various semiconductors, transparent heat-resistant materials, surface acoustic wave device substrates, and heat-resistant bath materials for molten metals. It has many uses. This aluminum nitride sintered body is generally manufactured by sintering aluminum nitride powder, but the properties of the obtained sintered body are greatly influenced by the purity and particle size of the raw material powder, and the high performance aluminum nitride sintered body In order to obtain a compact, it is required to use highly purified and fine aluminum nitride powder.

従来技術 従来の窒化アルミニウム粉末の製造法としては、(1)
金属アルミニウム粉を直接窒化する方法。
Prior Art Conventional methods for producing aluminum nitride powder include (1)
A method for directly nitriding metal aluminum powder.

(2)酸化アルミニウム粉を炭素還元窒化する方法。(2) A method of reducing and nitriding aluminum oxide powder with carbon.

(3)アルミニウムハライドとアンモニヤとの反応を利
用して気相合成する方法がある。
(3) There is a method of vapor phase synthesis using the reaction between aluminum halide and ammonia.

しかしながら、前記(1)、 (2)の方法では粒径1
μm以下の窒化アルミニウム粉を得ることが困難であり
、前記(3)の方法では高純度の窒化アルミニウム粉が
得難い欠点を有していた。これらの欠点を克服すべく、
本発明者らはさきに、全雰囲気中で熱処理すると容易に
窒化アルミニウムとなる。しかし、該混合粉中の金属ア
ルミニウムは極めて活性であるため、僅かな酸素によっ
て発火や酸化を生じたり、窒素雰囲気中の熱処理過程で
金属アルミニウム粉の焼結を生じ易いと言う問題点があ
った。
However, in the methods (1) and (2) above, the particle size 1
It is difficult to obtain aluminum nitride powder with a size of .mu.m or less, and the method (3) has the drawback that it is difficult to obtain highly pure aluminum nitride powder. In order to overcome these shortcomings,
The present inventors first conducted a heat treatment in a full atmosphere to easily form aluminum nitride. However, since the metal aluminum in the mixed powder is extremely active, there were problems in that a small amount of oxygen could cause ignition or oxidation, and the metal aluminum powder could easily sinter during the heat treatment process in a nitrogen atmosphere. .

発明の目的 本発明は前記問題点を解決すべくなされたもので、その
目的は金属アルミニウムの窒素プラズマ溶融により生成
する金属アルミニウムを窒化させ、窒化アルミニウム超
微粉とする方法を提供するにある。
OBJECTS OF THE INVENTION The present invention has been made to solve the above-mentioned problems, and its purpose is to provide a method for nitriding metal aluminum produced by nitrogen plasma melting of metal aluminum to produce ultrafine aluminum nitride powder.

発明の構成 本発明者らは前記目的を達成すべく鋭意研究の結果、金
属アルミニウムを窒素雰囲気中でアークまたはプラズマ
ジェットのフレームにより溶融して窒化アルミニウムと
金属アルミニウムの混合超微粉を製造する際、雰囲気中
にアンモニヤを共存させると、発生するアルミニウム蒸
気及びアルミニウム超微粉も窒化されて窒化アルミニウ
ムとなることを究明し得た。この知見に基いて本発明を
完成したものである。
Composition of the Invention As a result of intensive research to achieve the above object, the present inventors found that when producing a mixed ultrafine powder of aluminum nitride and metallic aluminum by melting metallic aluminum with an arc or plasma jet flame in a nitrogen atmosphere, It was found that when ammonia coexists in the atmosphere, the generated aluminum vapor and ultrafine aluminum powder are also nitrided to become aluminum nitride. The present invention was completed based on this knowledge.

本発明の要旨 アークまたはプラズマジェットのフレームにより金属ア
ルミニウムを溶融して超微粉を製造する際、雰囲気を窒
素とアンモニヤの混合ガスあるいは窒素とアンモニヤと
不活性ガスの混合ガスとすることを特徴とする窒化アル
ミニウム超微粉の製造法にある。
Summary of the present invention When producing ultrafine powder by melting metal aluminum with an arc or plasma jet flame, the atmosphere is a mixed gas of nitrogen and ammonia or a mixed gas of nitrogen, ammonia, and an inert gas. The method for producing ultrafine aluminum nitride powder.

本発明の方法における雰囲気中のアンモニヤ生成する。Ammonia production in the atmosphere in the method of the invention.

              し)−一一′二 NH,−、N鴇+H(1) NH,→NH+H(2) NH−N+H(3) これらの反応によって生成した活性化学種は、アルミニ
ウム蒸気あるいはその超微粉と容易に反応し、窒化アル
ミニウム超微粉を生成する。
) -11'2NH,-,N+H (1) NH,→NH+H (2) NH-N+H (3) The active chemical species generated by these reactions easily mix with aluminum vapor or its ultrafine powder. Reacts to produce ultrafine aluminum nitride powder.

すなわち、 NHs + A 1→AIN+H2(4)NH+Al→
A I N + 1/2Hs       (5)N 
+AL−4AIN          (6)一方(4
) (5)によって生成した水素は、本発明者らがさき
に発明した特許(第1146170号)に示すように、
金属アルミニウムの蒸気を発生させる要因となるもので
あり、そのためアンモニアのみの雰囲気を用いた場合に
は、アルミニウム蒸気に対する窒素の割合が減少し、超
微粉の窒化率が低下する。本発明におけるアンモニヤへ
の窒素の混入は、この不足する窒素の補充と共に反応(
1)〜(3)によって生成する活性な原子状水素と窒素
との反応、すなわち、 172N鵞+2H−NHt         (7)1
/2Nz + H−NH(8) によりNH,、NHの活性化学種を生成させる点にある
That is, NHs + A 1 → AIN + H2 (4) NH + Al →
A I N + 1/2Hs (5)N
+AL-4AIN (6) On the other hand (4
) The hydrogen produced by (5) is as shown in the patent (No. 1146170) invented by the present inventors,
This is a factor in generating metal aluminum vapor, so when an atmosphere containing only ammonia is used, the ratio of nitrogen to aluminum vapor decreases, and the nitriding rate of the ultrafine powder decreases. In the present invention, the mixing of nitrogen into ammonia is accompanied by a reaction (
The reaction between active atomic hydrogen and nitrogen produced by 1) to (3), i.e., 172N + 2H-NHt (7) 1
/2Nz + H-NH(8) to generate active chemical species of NH, NH.

このため、少なくとも雰囲気中に窒素とアンモニナを共
存させる必要がある。
For this reason, it is necessary to make at least nitrogen and ammonia coexist in the atmosphere.

その方法としては、 (1)窒素とアンモニヤの混合ガスあるいはこれを不活
性ガスで稀釈した混合ガスの雰囲中で発生したアークま
たはプラズマジェットのフレームにより金属アルミニウ
ムを溶融する方法。
The methods include: (1) A method of melting metal aluminum using an arc or plasma jet flame generated in an atmosphere of a mixed gas of nitrogen and ammonia or a mixed gas made by diluting this gas with an inert gas.

(2)窒素または窒素と不活性ガスの雰囲気中で発生さ
せたアークまたはプラズマジェットのフレームにより金
属アルミニウムを溶融させ、該溶融アルミニウムの周囲
にアンモニヤ、アンモニヤと窒素の混合ガス、あるいは
該混合ガスを不活性ガスで稀釈した気流を導入する方法
(2) Metal aluminum is melted by an arc or plasma jet flame generated in an atmosphere of nitrogen or nitrogen and an inert gas, and ammonia, a mixed gas of ammonia and nitrogen, or the mixed gas is placed around the molten aluminum. A method of introducing an air stream diluted with an inert gas.

がある。There is.

窒素とアンモニヤの混合割合は、N2とNH,の比が0
.01〜50の範囲、好ましくは0.1〜10である。
The mixing ratio of nitrogen and ammonia is such that the ratio of N2 and NH is 0.
.. The range is from 0.01 to 50, preferably from 0.1 to 10.

不活性ガスの混合割合は不活性ガスの割合が70容量係
以下であることが望ましい。雰囲本発明の方法における
プラズマ発生による超微粉を製造する装置としては、第
1図に示すものが挙げられる。lは放電電極用ガス入口
、2は旋回流雰囲気ガス入口、3はアークプラズマ、4
は溶融アルミニウム、5はハース、6は冷却器、7は捕
集器、8は密閉容器を示す。
The mixing ratio of the inert gas is preferably 70% by volume or less. Atmosphere An example of an apparatus for producing ultrafine powder by plasma generation in the method of the present invention is shown in FIG. l is a discharge electrode gas inlet, 2 is a swirling flow atmosphere gas inlet, 3 is an arc plasma, 4
5 indicates a molten aluminum, 5 indicates a hearth, 6 indicates a cooler, 7 indicates a collector, and 8 indicates a closed container.

実施例1 雰囲気に3O−N2 70チ(チは容量)の混合ガスを
使用し、全圧1気圧とし、該雰囲気中で直流アークプラ
ズマ(電流150A)を発生させて金属アルミニウムを
溶融させて窒化アルミニウム超微粉を得た。該超微粉の
電子顕微鏡写真は第2図の通りであった。該第2図が示
すように得られた窒化アルミニウム超微粉は種々の晶癖
を有する多面体であり、その最大径は約0.5μm以下
であった。
Example 1 A mixed gas of 3O-N2 70 cm (ch is capacity) was used in the atmosphere, the total pressure was 1 atm, and a DC arc plasma (current 150 A) was generated in the atmosphere to melt metal aluminum and nitride it. Ultrafine aluminum powder was obtained. An electron micrograph of the ultrafine powder was as shown in FIG. As shown in FIG. 2, the obtained ultrafine aluminum nitride powder was polyhedral with various crystal habits, and its maximum diameter was about 0.5 μm or less.

また、該超微粉の粉末X線回折図形を示すと第3図の通
りであった。該第3図形が示すように、ウルツ鉱型の窒
化アルミニウム単相から成り、金属アルミニウムの残留
は認められなかった。なお、その化学分析の結果、その
窒化率は98チ以上であった。
Furthermore, the powder X-ray diffraction pattern of the ultrafine powder was as shown in FIG. As shown in the third figure, it consisted of a single phase of wurtzite-type aluminum nitride, and no residual metallic aluminum was observed. As a result of chemical analysis, the nitriding rate was 98 or more.

実施例2 第1図に示す装置を用い、放電電極より窒素ガス(15
17m1n )を、アーク周囲の旋回流ガスとしてアン
モニヤ(30Q/min )をそれぞれ使用し、金属ア
ルミニウムを直流アークプラズマ(電流150A)で溶
融することにより窒化アルミニウム超微粉を得た。得ら
れた窒化アルミニウム超微粉の形体及び粒径は実施例1
とほぼ同一であった。
Example 2 Using the apparatus shown in Fig. 1, nitrogen gas (15
Ultrafine aluminum nitride powder was obtained by melting metal aluminum with direct current arc plasma (current 150 A) using ammonia (30 Q/min ) as a swirling gas around the arc. The shape and particle size of the obtained ultrafine aluminum nitride powder are those of Example 1.
was almost the same.

また、その粉末X線回折図形は第4図の通りであり、該
超微粉にはわずかの金属アルミニラ次の表の通りでその
純度は極めて高いものであ。
The powder X-ray diffraction pattern is as shown in Figure 4, and the ultrafine powder contains a small amount of metal aluminium, as shown in the table below, indicating that its purity is extremely high.

、−・ った。                  °−−−
AI Fe Si Mg Ca Mn Cu Ni C
o Ag Or W本発明超微粉 B  4  古+ 
古  −士 士 −一一一標準試料10よ±42±3去
+古士− (註)強度 −く古く士く士く+〈2・・・・・・〈1
0標準試料の組成(pT)m)  Fe : 20、H
g:5、Ag:2Ca:1、Si〈1、Cu(l、 Mn (1 発明の効果 本発明の方法tこよると、雰囲気にアンモニヤを窒素と
共存させることにより発生した金属アルミニウムを窒化
して窒化アルミニウムに転換し得られ、従来方法におけ
る金属アルミニウムと窒化アルミニウムの混合粉として
得られる欠点をなくし得た優れた効果を有する。
,-・ It was. °---
AI Fe Si Mg Ca Mn Cu Ni C
o Ag Or W Ultrafine powder of the present invention B 4 Old +
Ancient - Master - 111 Standard Sample 10 ± 42 ± 3 + Ancient Master - (Note) Strength - Ancient Master +〈2・・・・・・〈1
Composition of 0 standard sample (pT) m) Fe: 20, H
g:5, Ag:2Ca:1, Si〈1, Cu(l, Mn (1) Effects of the Invention The method of the present invention t Accordingly, metallic aluminum generated by coexisting ammonia with nitrogen in the atmosphere is nitrided. It has the excellent effect of eliminating the drawbacks of the conventional method of obtaining a mixed powder of metal aluminum and aluminum nitride.

【図面の簡単な説明】[Brief explanation of drawings]

第1図は本発明の方法を実施する装置の一実施態様図、
第2図は本発明の方法で得られる窒化アルミニウム超微
粉の電子顕微鏡写真、第3図及び第4図は本発明の方法
で得られる窒化アルミニウム超微粉の粉末X線回折図形
。 1:放電電極用ガス人口  2:旋回流雰囲気ガス入口
3:アークプラズマ  4:溶融アルミニウム5:ハー
ス      6:冷却器 7;捕集器      8:密閉容器 萌1図 第2図 第31】 54図
FIG. 1 is a diagram of an embodiment of an apparatus for carrying out the method of the present invention;
FIG. 2 is an electron micrograph of ultrafine aluminum nitride powder obtained by the method of the present invention, and FIGS. 3 and 4 are powder X-ray diffraction patterns of ultrafine aluminum nitride powder obtained by the method of the present invention. 1: Gas population for discharge electrode 2: Swirl flow atmosphere gas inlet 3: Arc plasma 4: Molten aluminum 5: Hearth 6: Cooler 7; Collector 8: Sealed container Moe 1 Figure 2 Figure 31] Figure 54

Claims (1)

【特許請求の範囲】 1)アークまたはプラズマジェットのフレームにより金
属アルミニウムを溶融して超微粉を製造する際、雰囲気
を窒素とアンモニヤの混合ガスあるいは窒素とアンモニ
ヤと不活性ガスの混合ガスとすることを特徴とする窒化
アルミニウム超微粉の製造法。 2)窒素とアンモニヤの混合ガスあるいは窒素とアンモ
ニヤと不活性ガスとの混合ガス雰囲中でアークまたはプ
ラズマジェットのフレームを発生させることにより雰囲
気を作ることからなる特許請求の範囲第1項記載の窒化
アルミニウム超微粉の製造法。 3)窒素あるいは窒素と不活性ガスとの混合ガスの雰囲
気中でアークまたはプラズマジェットのフレームを発生
させ、溶融アルミニウムの周囲にアンモニヤ、アンモニ
ヤと窒素との混合ガスまたはアンモニヤと窒素と不活性
ガスとの混合ガスを導入して雰囲気を作ることからなる
特許請求の範囲第1項記載の窒化アルミニウムの超微粉
の製造法。
[Claims] 1) When producing ultrafine powder by melting metallic aluminum with an arc or plasma jet flame, the atmosphere is a mixed gas of nitrogen and ammonia or a mixed gas of nitrogen, ammonia, and an inert gas. A method for producing ultrafine aluminum nitride powder characterized by: 2) The atmosphere is created by generating an arc or a plasma jet flame in a mixed gas atmosphere of nitrogen and ammonia or a mixed gas of nitrogen, ammonia, and an inert gas. A method for producing ultrafine aluminum nitride powder. 3) Generate an arc or plasma jet flame in an atmosphere of nitrogen or a mixture of nitrogen and an inert gas, and apply ammonia, a mixture of ammonia and nitrogen, or ammonia, nitrogen, and an inert gas around the molten aluminum. A method for producing ultrafine aluminum nitride powder according to claim 1, which comprises creating an atmosphere by introducing a mixed gas of.
JP12466686A 1986-05-31 1986-05-31 Production of extremely fine aluminum nitride powder Granted JPS62283805A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP12466686A JPS62283805A (en) 1986-05-31 1986-05-31 Production of extremely fine aluminum nitride powder

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP12466686A JPS62283805A (en) 1986-05-31 1986-05-31 Production of extremely fine aluminum nitride powder

Publications (2)

Publication Number Publication Date
JPS62283805A true JPS62283805A (en) 1987-12-09
JPH0460046B2 JPH0460046B2 (en) 1992-09-25

Family

ID=14891046

Family Applications (1)

Application Number Title Priority Date Filing Date
JP12466686A Granted JPS62283805A (en) 1986-05-31 1986-05-31 Production of extremely fine aluminum nitride powder

Country Status (1)

Country Link
JP (1) JPS62283805A (en)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5468697A (en) * 1993-03-16 1995-11-21 Yoshida Kogyo K.K. Composite ultrafine particles of aluminum nitride and rare earth nitride, method for production and sintered article thereof
US5549951A (en) * 1993-09-08 1996-08-27 Ykk Corporation Composite ultrafine particles of nitrides, method for production and sintered article thereof
WO2012115430A2 (en) * 2011-02-21 2012-08-30 서울대학교 산학협력단 Method for preparing aluminum/aluminum nitride or aluminum alloy/aluminum nitride composite materials

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS61174107A (en) * 1985-01-28 1986-08-05 High Frequency Heattreat Co Ltd Production of ultrafine aluminum nitride particle
JPS6241704A (en) * 1985-08-16 1987-02-23 Nec Corp Synthesis of aluminum nitride

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS61174107A (en) * 1985-01-28 1986-08-05 High Frequency Heattreat Co Ltd Production of ultrafine aluminum nitride particle
JPS6241704A (en) * 1985-08-16 1987-02-23 Nec Corp Synthesis of aluminum nitride

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5468697A (en) * 1993-03-16 1995-11-21 Yoshida Kogyo K.K. Composite ultrafine particles of aluminum nitride and rare earth nitride, method for production and sintered article thereof
US5549951A (en) * 1993-09-08 1996-08-27 Ykk Corporation Composite ultrafine particles of nitrides, method for production and sintered article thereof
WO2012115430A2 (en) * 2011-02-21 2012-08-30 서울대학교 산학협력단 Method for preparing aluminum/aluminum nitride or aluminum alloy/aluminum nitride composite materials
WO2012115430A3 (en) * 2011-02-21 2012-12-20 서울대학교 산학협력단 Method for preparing aluminum/aluminum nitride or aluminum alloy/aluminum nitride composite materials

Also Published As

Publication number Publication date
JPH0460046B2 (en) 1992-09-25

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