JPH0768043B2 - Method for producing ultrafine aluminum nitride particles - Google Patents
Method for producing ultrafine aluminum nitride particlesInfo
- Publication number
- JPH0768043B2 JPH0768043B2 JP22498686A JP22498686A JPH0768043B2 JP H0768043 B2 JPH0768043 B2 JP H0768043B2 JP 22498686 A JP22498686 A JP 22498686A JP 22498686 A JP22498686 A JP 22498686A JP H0768043 B2 JPH0768043 B2 JP H0768043B2
- Authority
- JP
- Japan
- Prior art keywords
- plasma
- gas
- aluminum nitride
- carrier gas
- ultrafine
- 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.)
- Expired - Fee Related
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Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J19/087—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
Description
【発明の詳細な説明】 （産業上の利用分野） 本発明は素材として優れた特性が注目され，利用が計ら
れようとしている，直径１μｍ以下の窒化アルミニウム
超微粒子の製造方法に関する。DETAILED DESCRIPTION OF THE INVENTION (Field of Industrial Application) The present invention relates to a method for producing ultrafine aluminum nitride particles having a diameter of 1 μm or less, which is attracting attention for its excellent properties as a material.
（従来の技術および問題点） 例えば、近着の金属材料技術研究所研究報告集７（1986
年報）掲載の論文『水素プラズマによる金属超微粒の製
造とその利用に関する研究』に見られる如く、近時、ア
ークまたはプラズマジエツトにより窒素を主成分とした
高温活性ガスを発生させ、当該高温活性ガスによつて各
種の金属を溶融・蒸発させ、窒化反応により金属窒化物
の超微粒子を得んとする試みがなされつつある。(Conventional Technology and Problems) For example, Research Report 7 (1986)
(Annual Report) As seen in the paper “Research on the production of ultrafine metal particles by hydrogen plasma and its utilization”, recently, high temperature active gas containing nitrogen as a main component was generated by arc or plasma jet, and the high temperature active gas was generated. Attempts are being made to melt and evaporate various metals with a gas and obtain ultrafine particles of metal nitride by a nitriding reaction.
ところで、上記論文第69頁の記載「金属あるいは窒化物
を出発物質とし,100％窒素ガスからなるアークプラズマ
により作成された超微粒子の組成は金属元素の種類によ
つて変化し、チタニウムやジルコニウムの場合には窒化
物超微粒子のみが得られ、アルミニウムの場合は金属ア
ルミニウムの超微粒子と窒化アルミニウム超微粒子との
混合物が得られ、また珪素の場合には珪素の超微粒子の
みが得られる」とし、かつ「上記現象は金属元素との新
和力の大小によつて影響を受ける結果と予想される」と
しているように、アルミニウムの窒化物超微粒子を得ん
とする場合には、金属アルミニウムの超微粒子の混入を
回避出来ないのが一般に認識されている現状である。By the way, the description on page 69 of the above-mentioned article "The composition of ultrafine particles produced by arc plasma consisting of a metal or a nitride as a starting material and consisting of 100% nitrogen gas changes depending on the kind of the metal element. In the case of aluminum, only ultrafine particles of nitride are obtained, in the case of aluminum, a mixture of ultrafine particles of metallic aluminum and ultrafine particles of aluminum nitride is obtained, and in the case of silicon, only ultrafine particles of silicon are obtained. '' Moreover, as described in "It is expected that the above-mentioned phenomenon will be influenced by the magnitude of the new force with the metallic element," when obtaining ultrafine aluminum nitride particles, At present, it is generally recognized that it is impossible to avoid mixing of fine particles.
しかし乍ら、本願出願人は上記文献（以下第１文献と云
う）の公開以前から高純度窒化アルミニウム超微粒子の
製造を目的として鋭意研究を進めており、当該第１文献
に先立ち、金属アルミニウムの混入がない高純度窒化ア
ルミニウム超微粒子の製造方法を発明し、昭和60年１月
28日付け特願昭60−12668号をもつて出願している。当
該先行発明の内容とするところは、雰囲気および高温プ
ラズマの成分を窒素，水素、または窒素と水素との化合
物、および必要に応じて添加される不活性ガスとし、高
周波エネルギーにより発生した高温プラズマフレームを
水冷ハース上の金属アルミニウム・バルクに作用させ、
当該金属アルミニウム・バルクからデンドライト（樹枝
状の結晶）を生成のうえ、当該デンドライトから溶融し
て蒸発する粒子が、高温反応性プラズマ中を通過して雰
囲気中へ拡散するようにして高純度の窒化アルミニウム
超微粒子を得るにある。However, the applicant of the present application has been earnestly researching for the purpose of producing high-purity aluminum nitride ultrafine particles before the publication of the above-mentioned document (hereinafter referred to as the first document). Invented a method for producing high-purity ultrafine aluminum nitride particles without contamination, January 1985
I am applying for Japanese Patent Application No. 60-12668 dated 28th. The content of the prior invention is that the atmosphere and the components of the high temperature plasma are nitrogen, hydrogen, or a compound of nitrogen and hydrogen, and an inert gas added as necessary, and the high temperature plasma flame generated by high frequency energy. Is applied to the metallic aluminum bulk on the water-cooled hearth,
After producing dendrites (dendritic crystals) from the metallic aluminum bulk, particles that melt and evaporate from the dendrites pass through the high temperature reactive plasma and diffuse into the atmosphere to obtain high-purity nitriding. To obtain ultrafine aluminum particles.
ところで、上記先行発明は高純度の窒化アルミニウム超
微粒子が得られるものの、デンドライトの生成とそれか
らの溶融・蒸発という２段階を経るため、生成速度が10
0gr/hrであつて、少量生産には適するものの、大量生産
には向かず、如何にして生産性を向上させるかが課題と
されていた。By the way, although the above-mentioned prior invention can obtain high-purity aluminum nitride ultrafine particles, it has a production rate of 10 because it undergoes two stages of production of dendrite and melting and evaporation from it.
Although 0 gr / hr was suitable for small-scale production, it was not suitable for mass production, and there was a problem how to improve productivity.
（発明に至る過程） 本発明者は、本発明を完成するに至る過程で各種の実験
を試みた。(Process leading to the invention) The present inventor tried various experiments in the process of completing the present invention.
第一に、前掲第１文献はアークプラズマを用いているの
で、本発明者は上記同様100％の窒素ガス成分を高周波
プラズマにより高温プラズマ化して金属アルミニウム・
バルクに作用させたところ、やはり第１文献とほぼ同様
の結果（金属アルミニウムの超微粒子70％，窒化アルミ
ニウムの超微粒子30％）を得た。当該実験結果から、10
0％の窒素ガス成分では高温プラズマ化エネルギー付与
手段の如何に拘わらず、得られる超微粒子に金属アルミ
ニウムの混入を回避し得ないことが確認されるととも
に、前掲先行発明における「窒素，水素、または窒素と
水素との化合物」を雰囲気および高温プラズマの成分と
することが的を得ていることが追認された。First, since the above-mentioned first document uses arc plasma, the present inventor, like the above, converts the 100% nitrogen gas component into high-temperature plasma by high-frequency plasma to form metallic aluminum.
When it was made to act on the bulk, almost the same results (70% of fine particles of metallic aluminum and 30% of ultrafine particles of aluminum nitride) were obtained as in the first document. From the experimental result, 10
It was confirmed that 0% nitrogen gas component could not avoid mixing of aluminum metal into the obtained ultrafine particles, regardless of the means for applying high temperature plasmaization energy, and the "nitrogen, hydrogen, or It was confirmed that it was appropriate to use "a compound of nitrogen and hydrogen" as a component of the atmosphere and high temperature plasma.
第二に、大量生産性を確保するためには、先行発明にお
ける，デンドライトの生成とそれからの溶融・蒸発とい
う２段階過程は不適当であり、金属アルミニウムを溶解
・蒸発させた蒸気から直接窒化物を得るようにすべきで
あるとの見解から、高周波エネルギにより高温プラズマ
化されるコアガス中に金属アルミニウムの粉末を載せて
キヤリアガスを兼務させる実験を行つた。当該実験は，
コアガスの成分条件ならびに粉末供給量を種々替えて行
つたにも拘わらず，それまで安定していた高周波プラズ
マがコアガス中に金属アルミニウム粉末を混入し始める
と直ちに消滅し、実験は不成功に終わつた。Secondly, in order to ensure mass productivity, the two-step process of producing dendrites and melting / evaporating the dendrites in the prior invention is unsuitable. From the viewpoint that it should be obtained, an experiment was conducted in which a powder of metallic aluminum was placed in a core gas that was turned into a high temperature plasma by high frequency energy so that the carrier gas also served as the carrier gas. The experiment is
The experiment was unsuccessful as soon as the high-frequency plasma, which had been stable until then, began mixing metal aluminum powder into the core gas, despite the fact that the component conditions of the core gas and the powder supply amount were changed. .
次いで、本発明者は金属アルミニウム粉末をコアガス以
外の輸送手段で高周波プラズマ中へ投入する方法を模索
した。当該方法は「1977年日本鉱業会秋季大会分科研究
会講演集；高周波プラズマによる粉体処理」（以下第２
文献と云う）に記載されている如く、粉体（純鉄）を高
周波プラズマ中へ自由落下させた場合,magnetic pumpin
g effectに起因して，殆どプラズマ中を通過せず、プラ
ズマの境界ではじきとばされてしまうので、従来から不
可能視されていた。Next, the present inventor sought a method of introducing metallic aluminum powder into high-frequency plasma by a transportation means other than the core gas. This method is described in "1977 Mining Society of Japan Autumn Meeting Subcommittee Study Meeting;
As described in (References), when powder (pure iron) is allowed to fall freely into high-frequency plasma, magnetic pumpin
Due to the g effect, it rarely passes through the plasma and is repelled at the boundaries of the plasma, so it has been considered impossible in the past.
然し、本発明者は上記現象の発生を克服すべく実験を重
ね、先行発明をさらに進展させて本発明をなすに至つ
た。However, the present inventor has conducted experiments to overcome the occurrence of the above phenomenon, and further advanced the prior invention to reach the present invention.
（発明の目的） 本発明は、高周波エネルギーを用いて金属アルミニウム
から窒化アルミニウム超微粒子を製造する場合の、先行
技術に存する問題点を解決し、かつ先行発明に存する課
題に応ずるためになされたもので、高純度の窒化アルミ
ニウム超微粒子を高い生産性をもつて製造可能な方法を
提供することを目的とする。(Object of the Invention) The present invention has been made in order to solve the problems existing in the prior art and to meet the problems existing in the prior invention when producing aluminum nitride ultrafine particles from metallic aluminum using high frequency energy. It is an object of the present invention to provide a method capable of producing high-purity ultrafine aluminum nitride particles with high productivity.
（発明の構成） 本発明の構成は、 （１）窒素を主たる成分とするガスを高周波エネルギー
により高温プラズマ化し金属アルミニウムに作用せしめ
て窒化アルミニウム超微粒子を得る場合において、 （２）金属アルミニウム粉末を含むキヤリアガスを上記
プラズマフレーム中に周方向から連続的に強制導入する
とともに、 （３）上記キヤリアガス導入後のプラズマフレーム中の
やや温度が低い周縁部へアンモニアガスを連続的に導入
するようにした ことを特徴とする窒化アルミニウム超微粒子の製造方法
にある。(Structure of the Invention) The structure of the present invention is (1) in the case where a gas containing nitrogen as a main component is subjected to high-temperature plasma generation by high-frequency energy to act on metal aluminum to obtain aluminum nitride ultrafine particles, (2) metal aluminum powder The carrier gas containing the gas is continuously and forcibly introduced into the plasma flame from the circumferential direction, and (3) the ammonia gas is continuously introduced to the peripheral portion of the plasma flame having a slightly low temperature after the introduction of the carrier gas. And a method for producing ultrafine aluminum nitride particles.
即ち、本発明は以下の２点を構成の特徴とするにある。That is, the present invention is characterized by the following two points.
前掲第２文献に見られるmagnetic pumping effectを
抑止するため、プラズマフレーム中に金属アルミニウム
粉末が含まれるキヤリアガスを周方向から連続的に強制
導入するように構成する。In order to suppress the magnetic pumping effect seen in the above-mentioned second document, a carrier gas containing metallic aluminum powder is continuously and forcibly introduced in the plasma frame in the circumferential direction.
前掲第１文献ならびに第１文献におけるアークプラズ
マを高周波プラズマに替えて行つた実験と先行発明との
対比考察から、金属アルミニウムが溶解・蒸発して生成
した蒸気はプラズマフレーム中心の10000K以上もある極
めて高温の領域では活性化した窒素と遭遇して窒化され
るが、逆に金属アルミニウムと窒素とに解離され易く、
言わば AlNAl＋Ｎ 現象を盛んに繰り返しており、AlN状態への定着はプラ
ズマ中でやや温度の低い周縁部で活性化してはいるもの
の、完全に分解していない窒素と水素との混合ガスない
し化合ガス中の窒素と遭遇し、逆現象が生じないでプラ
ズマフレーム外へ拡散すると判断され、当該判断に基ず
いて、金属アルミニウム粉末が必ずしもプラズマフレー
ム中心に達する必要はなく、溶解・蒸発する温度領域に
可及的長時間滞留すればよい構成、および蒸気がプラズ
マ中でやや温度の低い周縁部で活性化した窒素と遭遇す
る構成をとる。From the above-mentioned 1st document and the experiment conducted by replacing the arc plasma with the high-frequency plasma in the 1st document and the consideration of the comparison with the prior invention, the vapor generated by melting and evaporating the metallic aluminum is more than 10,000K at the center of the plasma flame. In the high temperature region, it encounters activated nitrogen and is nitrided, but on the contrary, it is easily dissociated into metallic aluminum and nitrogen,
In other words, the AlNAl + N phenomenon is repeatedly repeated, and although the fixing to the AlN state is activated in the peripheral part where the temperature is slightly lower in the plasma, it is not completely decomposed in the mixed gas of nitrogen and hydrogen or in the compound gas. It is judged that the metal aluminum powder diffuses out of the plasma flame without causing the reverse phenomenon, and based on this judgment, the metal aluminum powder does not necessarily have to reach the center of the plasma flame, and it can be formed in the temperature range where it melts and evaporates. The structure is such that it stays for as long as possible, and the structure in which the vapor encounters the activated nitrogen at the peripheral portion where the temperature is slightly low in the plasma.
（実施例） 本発明方法を第１図および第２図として示す一実施例に
従つて以下に詳述する。(Example) The method of the present invention will be described in detail below with reference to an example shown in FIGS. 1 and 2.
第１図は実施例装置の全体を示し、Chはチヤンバ,10は
チヤンバChの上部に配置された高周波高温プラズマ発生
装置,20は高周波高温プラズマ発生装置10とチヤンバCh
との間に配置された原料供給装置である。FIG. 1 shows the entire apparatus of the embodiment, where Ch is a chamber, 10 is a high frequency high temperature plasma generator placed above the chamber Ch, and 20 is a high frequency high temperature plasma generator 10 and a chamber Ch.
It is a raw material supply device arranged between and.
上記高周波高温プラズマ発生装置10は耐熱材製トーチ1
1,高周波電源Ｅおよび当該高周波電源Ｅに接続されるコ
イルＣとからなり、上記トーチ11は外管111および内管1
12として示す二重管で、外管111の一方端面が上記原料
供給装置20と接続して開口し、当該外管111の閉とされ
た他方端面を内管112が貫通して所定位置に開口してい
る。上記コイルＣは外管111の一重となつている外周に
卷回されている。上記トーチ11には、内管112の外管111
外とされている部分の，例えば閉端面に開口する導管12
から高温プラズマ発生用ガス（以下コアガスと云う）と
して窒素または窒素と不活性ガスである例えばアルゴン
との混合ガスG1が、また外管111の閉端面近傍に開口す
る導管13から当該外管111の管壁冷却用ガスとして窒素
ガスG2がそれぞれ導入可能に構成されている。The high-frequency high-temperature plasma generator 10 is a heat-resistant torch 1
1. A high frequency power source E and a coil C connected to the high frequency power source E. The torch 11 is an outer tube 111 and an inner tube 1.
In the double pipe shown as 12, one end face of the outer pipe 111 is connected to the raw material supply device 20 and opened, and the other end face of the outer pipe 111 is closed by the inner pipe 112 and opened at a predetermined position. is doing. The coil C is wound around the outer circumference of the outer pipe 111. The torch 11 includes an outer pipe 111 of an inner pipe 112.
Conduit 12 that opens to the outer end, for example, the closed end face
From which a high-temperature plasma generating gas (hereinafter referred to as a core gas) is nitrogen or a mixed gas G1 of nitrogen and an inert gas, for example, argon, and a conduit 13 opening near the closed end surface of the outer tube 111 from the outer tube 111. Nitrogen gas G2 can be introduced as a pipe wall cooling gas.
上記原料供給装置20は、本実施例では内径を前記外管11
1の内径と同径とした環状管部材からなり、管内は軸線
直角方向の仕切り壁21により室2Aおよび2Bに区画されて
いる。室2Aは，第２図に示される如く，内周壁に複数の
貫通孔s1が孔設されており、かつ室内に導管22を介して
金属アルミニウム粉末を載せて輸送するキヤリアガスG3
……例えば窒素ガスを供給可能である。而して、上記複
数の貫通孔s1それぞれは外管111内に発生するＰとして
示す高周波高温プラズマフレーム（以下プラズマフレー
ムと云う）の接線方向，もしくは接線方向より所定角度
範囲中心向き方向を指向する如く所定間隔を隔てる内周
壁を同一向きに斜めに貫通している。室2Bも室2A同様内
周壁に複数の貫通孔s2が孔設されており、かつ室内に導
管23を介してアンモニアガスG4を供給可能である。而し
て、上記複数の貫通孔s2それぞれは前記貫通孔s1と同じ
向きでプラズマフレームＰの接線方向を指向する如く内
周壁を斜めに貫通している。In the present embodiment, the raw material supply device 20 has an inner diameter of the outer tube 11
The inside of the pipe is divided into chambers 2A and 2B by a partition wall 21 perpendicular to the axis. As shown in FIG. 2, the chamber 2A has a plurality of through holes s1 formed in the inner peripheral wall thereof, and a carrier gas G3 for carrying metallic aluminum powder on the chamber via a conduit 22 for transporting the powder.
...... For example, nitrogen gas can be supplied. Thus, each of the plurality of through holes s1 is directed in a tangential direction of a high-frequency high-temperature plasma frame (hereinafter referred to as a plasma frame) indicated by P generated in the outer tube 111, or in a direction toward a center of a predetermined angle range from the tangential direction. As described above, the inner peripheral walls that are separated by a predetermined distance are obliquely penetrated in the same direction. Similarly to the chamber 2A, the chamber 2B has a plurality of through holes s2 formed in the inner peripheral wall thereof, and the ammonia gas G4 can be supplied into the chamber via the conduit 23. Thus, each of the plurality of through holes s2 obliquely penetrates the inner peripheral wall in the same direction as the through hole s1 so as to point in the tangential direction of the plasma frame P.
上記チヤンバChの所定位置には導管３の一方端が開口し
ており、当該導管３の他方端はフイルタ41を備えた捕集
器４を介して図示しないガス吸引装置に接続されてい
る。One end of the conduit 3 is open at a predetermined position of the chamber Ch, and the other end of the conduit 3 is connected to a gas suction device (not shown) via a collector 4 equipped with a filter 41.
以上の構成からなる装置を用いて、窒化アルミニウムの
超微粒子を製造する場合を以下に述べる。A case of producing ultrafine particles of aluminum nitride using the apparatus having the above configuration will be described below.
先ずガス吸引装置を駆動させてチヤンバCh内の空気を排
出し、代わりに導管12からコアガスG1を流入してチヤン
バCh内に雰囲気を形成する。次いで高周波電源Ｅを投入
して誘導コイルＣに通電する。コアガスG1はコイルＣが
外周に卷回されている外管111内高周波エネルギー付与
領域において点火され、高温プラズマ化する。同時にガ
スG2を導管13から導入して外管111の管壁の冷却を開始
する。プラズマフレームＰの安定を確認のうえ、原料供
給装置20の室2Aへは定量の金属アルミニウム粉末を載せ
たキヤリヤガスG3を，また室2BへはアンモニアガスG4
を，それぞれ所定の流量に従つて供給する。First, the gas suction device is driven to discharge the air in the chamber Ch, and instead, the core gas G1 is introduced from the conduit 12 to form an atmosphere in the chamber Ch. Next, the high frequency power source E is turned on to energize the induction coil C. The core gas G1 is ignited in the high frequency energy application region in the outer tube 111 where the coil C is wound around the outer circumference, and is turned into high temperature plasma. At the same time, the gas G2 is introduced from the conduit 13 to start cooling the tube wall of the outer tube 111. After confirming the stability of the plasma flame P, a carrier gas G3 containing a fixed amount of metallic aluminum powder is placed in the chamber 2A of the raw material supply device 20, and an ammonia gas G4 is placed in the chamber 2B.
Are supplied according to the respective predetermined flow rates.
室2Aへ供給されたキヤリヤガスG3は複数の貫通孔s1から
プラズマフレームＰの接線方向，もしくは接線方向より
所定角度範囲中心向き方向を指向して噴出し、プラズマ
フレームＰの周囲に方向性をもつた渦流を形成する。当
該渦流の内側は複数の貫通孔s1から後続するキヤリヤガ
スG3の噴出流に押されてプラズマフレームＰの中心方向
へと順次移動し、キヤリヤガスG3に載さられている金属
アルミニウム粉末は高温域（必ずしもプラズマフレーム
Ｐの中心域ではない）を渦流に従つて浮遊状態で周回移
動することとなる。この場合、後続するキヤリヤガスG3
の噴出流がmagnetic pumping effectを抑止し、金属ア
ルミニウム粉末がプラズマフレームＰ外にはじき飛ばさ
れる虞はない。The carrier gas G3 supplied to the chamber 2A is jetted from a plurality of through holes s1 in the tangential direction of the plasma frame P or in the direction toward the center of a predetermined angle range from the tangential direction, and has a directivity around the plasma frame P. Form a vortex. The inside of the vortex is pushed by the subsequent jets of carrier gas G3 from the plurality of through holes s1 and sequentially moves toward the center of the plasma frame P, and the metallic aluminum powder placed on the carrier gas G3 is heated to a high temperature region (not necessarily The plasma frame P (not in the central region) is orbitally moved in a floating state according to the vortex flow. In this case, the subsequent carrier gas G3
Of the metal aluminum powder suppresses the magnetic pumping effect, and there is no possibility that the metal aluminum powder is repelled to the outside of the plasma frame P.
高温のプラズマフレームＰ内を渦流に従つて浮遊する金
属アルミニウム粉末は溶解・蒸発して金属蒸気となり、
活性化された窒素と盛んに結合・解離を繰り返しつつ次
第に集合して下降する。下降する超微粒子は、直ちに室
2Bへ供給され，プラズマフレームＰ中のやや低温の周縁
部に接線方向を指向して噴出する如く導入されたアンモ
ニアガスG4の噴出流により渦流が形成され、かつプラズ
マフレームＰの高温により温度が十分上昇している領域
に達し、活性化してはいるものの，完全に窒素と水素と
に分解してはいない窒素と遭遇して窒化され、当該状態
を維持したままプラズマフレームＰ外へと拡散する。The metallic aluminum powder floating in the high-temperature plasma frame P according to the vortex is melted and evaporated to become metallic vapor,
It gradually aggregates and descends while repeatedly binding and dissociating with activated nitrogen. The ultrafine particles that descend are immediately
2B, a vortex is formed by the jet flow of the ammonia gas G4 that is introduced so as to be jetted in a tangential direction to the peripheral portion of the plasma flame P having a slightly low temperature, and the temperature is sufficiently high due to the high temperature of the plasma flame P. It reaches the rising region and encounters nitrogen which has been activated but has not been completely decomposed into nitrogen and hydrogen, is nitrided, and diffuses outside the plasma flame P while maintaining the state.
チヤンバCh内に拡散した窒化アルミニウムの超微粒子の
一部は諸ガスともども作動中の吸引装置により導管３へ
と吸引され、捕集器４のフイルタ41に捕獲され、一部は
チヤンバCh内壁と導管３の管壁に付着する。A part of the ultrafine particles of aluminum nitride diffused in the chamber Ch is sucked into the conduit 3 by the suction device in operation together with various gases and captured by the filter 41 of the collector 4, and a part of the inner wall of the chamber Ch and the conduit 41. Adhere to the tube wall of No. 3.
尚、チヤンバCh内の雰囲気ガス圧は、プラズマフレーム
Ｐが安定して得られる圧力とされればよく、例えば常
圧、下限は通常400Torr程度である。The atmospheric gas pressure in the chamber Ch may be a pressure at which the plasma flame P can be stably obtained. For example, the atmospheric pressure, the lower limit is usually about 400 Torr.
（実験例） 本発明者が行つた実験例を以下に示す。(Experimental Example) An experimental example conducted by the present inventor is shown below.
☆使用装置；第１図に示す装置を使用した。☆ Device used: The device shown in Fig. 1 was used.
☆電源；周波数……4MHz 出 力……35KW ☆原料；金属アルミニウム粉末 純度……99.98％ ☆実験方法；第１図に示す装置を使用し、ガスG1,G2,G3
およびG4それぞれの流量とガスG3に載せる原料粉末とを
下記の如く設定して窒化アルミニウム超微粒子を製造す
る実験を実施した。☆ Power supply: Frequency: 4MHz Output: 35KW ☆ Raw material: Metal aluminum powder Purity: 99.98% ☆ Experimental method: Gas G1, G2, G3 using the device shown in Fig. 1.
An experiment for producing aluminum nitride ultrafine particles was carried out by setting the respective flow rates of G4 and G4 and the raw material powder to be placed in the gas G3 as follows.
○コアガスG1:Ar……18/min N2……15/min ○冷却ガスG2:N2……21/min ○キヤリヤガスG3: N2…５/min 原料粉末……約10g/min （約600g/hr） ○アンモニアガス（NH3）G4:……20/min ☆結果；捕集器４のフイルタ41に捕獲された超微粒子お
よびチヤンバChの内壁と導管３の管壁に付着した超微粒
子とを掻き落とし、総重量を計測したところ、原料粉末
重量とほぼ等しい超微粒子が得られた。○ Core gas G1: Ar …… 18 / min N 2 …… 15 / min ○ Cooling gas G2: N 2 …… 21 / min ○ Carrier gas G3: N 2 … 5 / min Raw material powder …… about 10g / min (about 600g / hr) ○ Ammonia gas (NH 3 ) G4: ...... 20 / min ☆ Results: Ultrafine particles captured by the filter 41 of the collector 4 and ultrafine particles adhering to the inner wall of the chamber Ch and the tube wall of the conduit 3. When scraped off and the total weight was measured, ultrafine particles approximately equal to the weight of the raw material powder were obtained.
また、得られた超微粒子をＸ線回折試験に付して純度を
調査したところ、極めて高純度の窒化アルミニウム超微
粒子が生成していることが確認された。Further, when the obtained ultrafine particles were subjected to an X-ray diffraction test to examine the purity, it was confirmed that extremely high-purity aluminum nitride ultrafine particles were produced.
（発明の作用） 本発明は、キヤリヤガスG3をmagnetic pumping effect
を抑制する如く噴出させてプラズマフレームＰ中に強制
導入する作用、当該キヤリヤガスG3に載せられている金
属アルミニウム粉末を高温域に可及的に長時間浮遊させ
て溶解・蒸発させて金属蒸気とする作用、当該金属蒸気
が活性化された窒素と盛んに結合と解離を繰り返しつつ
次第に集合して微粒子となつて下降しプラズマフレーム
Ｐ外へと拡散する過程で活性化してはいるものの，完全
に窒素と水素とに分解してはいないアンモニアガスG4中
の窒素に遭遇して窒化，かつ当該状態を維持したままプ
ラズマフレームＰ外へ拡散せしめる作用がある。(Effect of the Invention) The present invention uses the carrier gas G3 with the magnetic pumping effect.
The effect of ejecting so as to suppress the gas and forcibly introducing it into the plasma flame P, the metallic aluminum powder placed on the carrier gas G3 is suspended in the high temperature region as long as possible to be melted and evaporated to form a metallic vapor. Although the metal vapor is activated in the process in which the metal vapor actively aggregates with the activated nitrogen and gradually dissociates, gradually aggregates into fine particles, descends, and diffuses to the outside of the plasma flame P, but the nitrogen is completely activated. There is an action of encountering nitrogen in the ammonia gas G4 which is not decomposed into hydrogen and hydrogen, nitriding, and diffusing it outside the plasma flame P while maintaining the state.
（他の実施例） 上記実施例ならびに実験例では、コアガスG1をアルゴン
と窒素の混合ガスとした場合を挙げて説明したが、コイ
ルＣの整合が良好でプラズマフレームＰの安定が得られ
るならば、原料供給装置20へのキヤリヤガスG3およびア
ンモニアガスG4供給に先立つて、高価なアルゴンガス含
有％を順次減らし、コアガスG1を窒素ガス100％とする
ことも可能であり、ランニングコスト低減に大きく貢献
することが可能となる。(Other Examples) In the above examples and experimental examples, the case where the core gas G1 is a mixed gas of argon and nitrogen was described, but if the matching of the coil C is good and the plasma flame P is stable, Prior to supplying the carrier gas G3 and the ammonia gas G4 to the raw material supply device 20, it is possible to sequentially reduce the expensive argon gas content% and the core gas G1 to 100% nitrogen gas, which greatly contributes to the reduction of the running cost. It becomes possible.
また実施例ならびに実験例では、キヤリヤガスG3を窒素
とした場合を挙げて説明したが、その成分はアンモニア
ガスあるいはアルゴンその他の不活性ガスでも良く、プ
ラズマフレームＰの安定のためには可及的にプラズマ化
し易いガスの使用が望ましく、かつプラズマフレームＰ
の安定が得られるならば、可及的に低廉なガスの使用が
望ましく、結論としてキヤリヤガスG3の種類を問うもの
ではない。Further, in the examples and the experimental examples, the case where the carrier gas G3 is nitrogen has been described, but the component may be ammonia gas, argon or other inert gas, and it is possible to stabilize the plasma flame P as much as possible. It is desirable to use a gas that is easily turned into plasma, and the plasma flame P
If stable gas is obtained, it is desirable to use the cheapest possible gas, and in conclusion, it does not matter what kind of carrier gas G3.
さらに上記実施例ならびに実験例では、環状管部材から
なる原料供給装置20を設けた場合を挙げて説明したが、
プラズマフレームＰ中にキヤリヤガスG3を強制導入可能
な構成、およびプラズマフレームＰ中の周縁部にアンモ
ニアガスG4を導入可能な構成を用いるならば、本発明と
同様な作用および当該作用から同一の効果が得られるの
で、その構造の如何にを問わず本発明の設計事項の範囲
に属すこと勿論である。Furthermore, in the above-mentioned Examples and Experimental Examples, the case where the raw material supply device 20 made of an annular pipe member was provided was described,
If a structure that can forcibly introduce the carrier gas G3 into the plasma flame P and a structure that can introduce the ammonia gas G4 into the peripheral edge of the plasma flame P are used, the same effect as the present invention and the same effect from the same effect can be obtained. Since it is obtained, it goes without saying that regardless of its structure, it belongs to the scope of design matters of the present invention.
（発明の効果） 本発明によれば、高純度の窒化アルミニウム超微粒子
を、先行発明に従つた場合の生産量に比し６倍以上の高
効率で製造可能となり、これにより生産コストが大幅に
低減され、従つて多くの産業分野で当該素材の具える優
れた性質を安価かつ豊富に活用出来ることとなり、本発
明からされる効果は甚大である。(Effect of the Invention) According to the present invention, high-purity aluminum nitride ultrafine particles can be produced with a high efficiency of 6 times or more as compared with the production amount according to the prior invention, which significantly reduces the production cost. Therefore, the excellent properties of the material can be utilized cheaply and abundantly in many industrial fields, and the effect of the present invention is great.
第１図は本発明方法の一実施例装置を示す断面正面図、
第２図は第１図におけるＸ−Ｘ線平面断面である。FIG. 1 is a sectional front view showing an apparatus according to an embodiment of the present invention,
FIG. 2 is a plane cross section taken along the line XX in FIG.
Claims (4)
ルギーにより高温プラズマ化し金属アルミニウムに作用
せしめて窒化アルミニウム超微粒子を得る場合におい
て、金属アルミニウム粉末を含むキヤリアガスを上記プ
ラズマフレーム中に周方向から連続的に強制導入すると
ともに、上記キヤリアガス導入後のプラズマフレーム中
のやや温度が低い周縁部へアンモニアガスを連続的に導
入するようにしたことを特徴とする窒化アルミニウム超
微粒子の製造方法。1. When a gas containing nitrogen as a main component is plasma-heated by high-frequency energy to act on metal aluminum to obtain aluminum nitride ultrafine particles, a carrier gas containing metal aluminum powder is continuously supplied in the plasma frame from the circumferential direction. The method for producing aluminum nitride ultrafine particles is characterized in that the ammonia gas is continuously forcibly introduced and the ammonia gas is continuously introduced to the peripheral portion of the plasma flame after the introduction of the carrier gas and having a slightly low temperature.
スである特許請求の範囲第１項記載の窒化アルミニウム
超微粒子の製造方法。2. The method for producing ultrafine aluminum nitride particles according to claim 1, wherein the carrier gas component is a gas that is easily turned into plasma.
アガスの指向方向が当該プラズマフレームの周囲に等間
隔を隔てて同一向きとした複数の接線方向，もしくは接
線方向より所定角度範囲中心向きである特許請求の範囲
第１項記載の窒化アルミニウム超微粒子の製造方法。3. The direction of the carrier gas forcibly introduced into the plasma frame is a plurality of tangential directions in which the same direction is provided at equal intervals around the plasma frame, or a direction toward the center of a predetermined angle range from the tangential direction. 2. The method for producing ultrafine aluminum nitride particles according to claim 1.
モニアガスの指向方向が当該プラズマフレームの周囲に
等間隔を隔て，かつキヤリアガスの指向方向と同一向き
とした複数の接線方向である特許請求の範囲第１項記載
の窒化アルミニウム超微粒子の製造方法。4. The direction of the ammonia gas introduced to the peripheral portion of the plasma frame is a plurality of tangential directions at equal intervals around the plasma frame and in the same direction as the direction of the carrier gas. The method for producing ultrafine aluminum nitride particles according to item 1.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP22498686A JPH0768043B2 (en) | 1986-09-25 | 1986-09-25 | Method for producing ultrafine aluminum nitride particles |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP22498686A JPH0768043B2 (en) | 1986-09-25 | 1986-09-25 | Method for producing ultrafine aluminum nitride particles |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS6385007A JPS6385007A (en) | 1988-04-15 |
| JPH0768043B2 true JPH0768043B2 (en) | 1995-07-26 |
Family
ID=16822305
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP22498686A Expired - Fee Related JPH0768043B2 (en) | 1986-09-25 | 1986-09-25 | Method for producing ultrafine aluminum nitride particles |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0768043B2 (en) |
Families Citing this family (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP4729180B2 (en) * | 2001-02-02 | 2011-07-20 | 株式会社茨木研究所 | Method for producing aluminum nitride |
| JP4545357B2 (en) * | 2001-07-23 | 2010-09-15 | 電気化学工業株式会社 | Method for producing aluminum nitride powder |
| JP4095272B2 (en) * | 2001-09-25 | 2008-06-04 | 株式会社東芝 | Fine particle production method and fine particle production apparatus |
| JP5136139B2 (en) | 2007-03-20 | 2013-02-06 | 東レ株式会社 | Black resin composition for resin black matrix, resin black matrix, color filter and liquid crystal display device |
| JP5824906B2 (en) * | 2011-06-24 | 2015-12-02 | 昭栄化学工業株式会社 | Plasma device for producing metal powder and method for producing metal powder |
| JP5954470B2 (en) * | 2015-06-26 | 2016-07-20 | 昭栄化学工業株式会社 | Plasma device for producing metal powder and method for producing metal powder |
| JP7016403B2 (en) | 2018-03-13 | 2022-02-04 | 富士フイルム株式会社 | Manufacturing method of cured film, manufacturing method of solid-state image sensor |
-
1986
- 1986-09-25 JP JP22498686A patent/JPH0768043B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPS6385007A (en) | 1988-04-15 |
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