JPS6351966B2 - - Google Patents
Info
- Publication number
- JPS6351966B2 JPS6351966B2 JP58185188A JP18518883A JPS6351966B2 JP S6351966 B2 JPS6351966 B2 JP S6351966B2 JP 58185188 A JP58185188 A JP 58185188A JP 18518883 A JP18518883 A JP 18518883A JP S6351966 B2 JPS6351966 B2 JP S6351966B2
- Authority
- JP
- Japan
- Prior art keywords
- powder
- reaction zone
- spherical
- sic
- melting point
- 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
Links
- 239000000843 powder Substances 0.000 claims description 35
- 238000006243 chemical reaction Methods 0.000 claims description 26
- 238000002844 melting Methods 0.000 claims description 13
- 230000008018 melting Effects 0.000 claims description 13
- 238000004519 manufacturing process Methods 0.000 claims description 7
- 238000009835 boiling Methods 0.000 claims description 6
- 150000001722 carbon compounds Chemical class 0.000 claims description 6
- 150000001875 compounds Chemical class 0.000 claims description 4
- 239000007789 gas Substances 0.000 description 8
- 238000010438 heat treatment Methods 0.000 description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 238000003917 TEM image Methods 0.000 description 4
- 229910052799 carbon Inorganic materials 0.000 description 4
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 description 2
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 2
- 229910004298 SiO 2 Inorganic materials 0.000 description 2
- 238000010000 carbonizing Methods 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000000155 melt Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000012071 phase Substances 0.000 description 2
- 239000011863 silicon-based powder Substances 0.000 description 2
- 238000003746 solid phase reaction Methods 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 239000005046 Chlorosilane Substances 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- 239000005977 Ethylene Substances 0.000 description 1
- 229910003902 SiCl 4 Inorganic materials 0.000 description 1
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- -1 but conventionally Substances 0.000 description 1
- 239000001273 butane Substances 0.000 description 1
- 238000003763 carbonization Methods 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- KOPOQZFJUQMUML-UHFFFAOYSA-N chlorosilane Chemical compound Cl[SiH3] KOPOQZFJUQMUML-UHFFFAOYSA-N 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 1
- 238000010574 gas phase reaction Methods 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 230000006698 induction Effects 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 238000004093 laser heating Methods 0.000 description 1
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 1
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000011224 oxide ceramic Substances 0.000 description 1
- 229910052574 oxide ceramic Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 238000005192 partition Methods 0.000 description 1
- 239000001294 propane Substances 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 238000001308 synthesis method Methods 0.000 description 1
Description
【発明の詳細な説明】
（産業上の利用分野）
本発明はSiC焼結体等の原料となるSiC粉末の
製造法に関するものである。詳しくは、気相反応
域にて融体化かつ微細球状化したSiを生成させ、
これを炭化することによる球状SiC粉末の製造法
に関するものである。DETAILED DESCRIPTION OF THE INVENTION (Field of Industrial Application) The present invention relates to a method for producing SiC powder, which is a raw material for SiC sintered bodies and the like. Specifically, we generate molten and finely spheroidized Si in the gas phase reaction zone,
This invention relates to a method for producing spherical SiC powder by carbonizing it.
（従来技術）
一般にセラミツクス焼結体の原料となる粉末の
形状はより球形に近い方が好ましいとされてい
る。これは球状粉末を用いた方が、焼結体や焼結
前の成形体の内部組織を均一にでき、ひいてはセ
ラミツクス焼結体の強度を改善できるからであ
る。そこで球状粉末を得ることが必要なのである
が、従来、酸化物系セラミツクス粉末、例えば
SiO2粉末やAl2O3粉末等では、これらを融点以上
の高温域に導入し、融体とし、その表面張力を利
用して球状化していた。(Prior Art) Generally, it is said that it is preferable that the shape of the powder serving as a raw material for a ceramic sintered body be closer to a spherical shape. This is because the use of spherical powder makes it possible to make the internal structure of the sintered body and the compact before sintering more uniform, thereby improving the strength of the ceramic sintered body. Therefore, it is necessary to obtain spherical powder, but conventionally, oxide ceramic powder, e.g.
In the case of SiO 2 powder, Al 2 O 3 powder, etc., these were introduced into a high temperature range above the melting point to form a melt, and the surface tension of the powder was used to form spheres.
しかしSiCのように通常融点を持たず、つまり
高温に加熱しても融体化せず気化してしまうもの
は前述のような従来の方法では球状化は不可能で
ある。又通常のSiC粉末の製造法、例えば、SiC
粗粉末の粉砕、Si粉末とＣ粉末の固相反応、Siの
酸化物粉末とＣ粉末の固相反応、従来のSi源とＣ
源を同一の反応域に導入する気相熱分解法および
気相合成法等では、真に球状と言える程のSiC粉
末を製造するのは困難であつた。 However, materials such as SiC that do not normally have a melting point, that is, they do not melt but vaporize even when heated to high temperatures, cannot be made into spheroids using the conventional methods described above. Also, regular SiC powder manufacturing methods, such as SiC
Grinding of coarse powder, solid phase reaction between Si powder and C powder, solid phase reaction between Si oxide powder and C powder, conventional Si source and C
It has been difficult to produce truly spherical SiC powder using gas phase pyrolysis and gas phase synthesis methods in which sources are introduced into the same reaction zone.
（発明の目的）
本発明は上述の欠点を改善したもので、球状
SiC粉末を得ることを目的としたものである。(Object of the invention) The present invention improves the above-mentioned drawbacks, and has a spherical shape.
The purpose is to obtain SiC powder.
（発明の構成）
本発明はSiCの構成元素であるSiをその融点
（1685K；JANAF'71）以上の第１反応域中にて
生成させ、これを融体として、その表面張力を利
用して球状化し、これをSiの融点以上沸点
（3492K；JANAF'71）以下の第２反応域にて、
炭素化合物と反応させ、球状SiC粉末を得ること
を特徴とする。(Structure of the Invention) The present invention generates Si, which is a constituent element of SiC, in the first reaction zone at a temperature higher than its melting point (1685K; JANAF'71), and uses the surface tension of the Si as a melt. It is spheroidized and then heated in a second reaction zone above the melting point of Si and below the boiling point (3492K; JANAF'71).
It is characterized by reacting with a carbon compound to obtain spherical SiC powder.
なおJANAFとは、種々の熱力学データを
JANAF THERMOCHEMICAL TABLES（米
国政府刊行物〔PB REPORT〕）として公表され
たものである。 JANAF refers to the collection of various thermodynamic data.
It was published as JANAF THERMOCHEMICAL TABLES (US government publication [PB REPORT]).
以下本発明の詳細を図面に基づいて説明する。 The details of the present invention will be explained below based on the drawings.
第１図は本発明で目的とする球状SiC粉末を製
造するための装置の断面図の一例である。これは
直流プラズマを利用し高温を発生させる反応装置
であるが、本発明において高温の発生方法はこれ
に限定されるものではない。第１図の装置では陰
極１と陽極２の間で放電させ、プラズマ用ガス導
入管３から導入したプラズマ用ガスをプラズマ化
し、第１反応域４にSiの融点以上の高温を発生さ
せる。ここへSi導入管５よりＣを含まないSi化合
物を導入し、融体化かつ微細球化したSiを生成さ
せる。このSiはプラズマ用ガスの流れにより第２
反応域６へ運ばれ、炭素導入管７より導入された
炭素化合物と反応し、球状SiC粉末が生成され
る。この時第２反応域６がSiの融点以上沸点以下
に保たれていることが重要である。これは融体化
かつ微細球状化したSiを炭化する際、その１粒に
注目すると、完全に炭化が終り、球状SiC粉末と
なるまでは、未反応のSi部は融体化したままの状
態が必要だからである。 FIG. 1 is an example of a sectional view of an apparatus for producing spherical SiC powder, which is the object of the present invention. Although this is a reaction device that generates high temperature using direct current plasma, the method of generating high temperature in the present invention is not limited to this. In the apparatus shown in FIG. 1, a discharge is caused between a cathode 1 and an anode 2, the plasma gas introduced from the plasma gas introduction tube 3 is turned into plasma, and a high temperature higher than the melting point of Si is generated in the first reaction zone 4. A C-free Si compound is introduced from the Si introduction pipe 5 to produce molten and finely spheroidized Si. This Si is transferred to the second layer by the flow of plasma gas.
It is transported to the reaction zone 6 and reacts with the carbon compound introduced through the carbon introduction tube 7 to produce spherical SiC powder. At this time, it is important that the second reaction zone 6 is maintained at a temperature above the melting point and below the boiling point of Si. This is because when carbonizing Si that has been molten and made into fine spherules, if you focus on a single particle, the unreacted Si portion remains molten until carbonization is complete and a spherical SiC powder is formed. This is because it is necessary.
こうして製造された球状SiC粉末は粉末取出口
８より取り出される。 The spherical SiC powder thus produced is taken out from the powder outlet 8.
第２図は直流プラズマの代わりに外部電気炉９
により第１反応域４をSiの融点以上に、第２反応
域をSiの融点以上沸点以下に保つ反応装置の例で
ある。球状SiC粉末の製造法は第１図の場合と同
様であり、Si導入管５より不活性ガス又はH2等
のキヤリアーガスとＣを含まないSi化合物を導入
し、炭素導入管７から炭素化合物を導入し、粉末
取り出し口８より球状SiC粉末を取り出す。原料
としては、Si化合物ではSiH4、塩化シラン、
SiCl4等が、炭素化合物としてはメタン、アセチ
レン、エチレン、プロパン、ブタン、ベンゼン、
ナフタリンなどの炭化水素等を用いることができ
る。 Figure 2 shows an external electric furnace 9 instead of DC plasma.
This is an example of a reactor in which the first reaction zone 4 is maintained at a temperature above the melting point of Si, and the second reaction zone is maintained at a temperature above the melting point of Si and below the boiling point. The method for producing spherical SiC powder is the same as that shown in Fig. 1, in which an inert gas or a carrier gas such as H 2 and a Si compound containing no C are introduced from the Si introduction tube 5, and a carbon compound is introduced from the carbon introduction tube 7. is introduced, and the spherical SiC powder is taken out from the powder take-out port 8. As raw materials, Si compounds include SiH 4 , chlorosilane,
SiCl 4 etc. are carbon compounds such as methane, acetylene, ethylene, propane, butane, benzene,
Hydrocarbons such as naphthalene can be used.
反応装置は第１図、第２図に限らず、第１反応
域をSiの融点以上に保つことができ、ここでは融
体化かつ微細球状化したSiが生成され、第２反応
域をSiの融点以上沸点以下に保つことができ、こ
こで該Siを炭化し球状SiC粉末が得られるもので
あれば、どのようなものでもよい。したがつて第
１反応域の加熱法は、高周波プラズマ、誘導加
熱、マイクロ波加熱、赤外線加熱、レーザー加熱
等いかなる加熱法でもよい。第２反応域において
もいかなる加熱法でも良く、さらに加熱せずとも
Siの融点以上沸点以下に保たれるならば加熱は不
要であり、又逆に冷却が必要なこともある。 The reactor is not limited to those shown in Figures 1 and 2, and can maintain the first reaction zone above the melting point of Si, where molten and fine spheroidal Si is produced, and the second reaction zone is heated to Si. Any material may be used as long as it can be maintained at a temperature above the melting point and below the boiling point of SiC, and where the Si can be carbonized to obtain spherical SiC powder. Therefore, the first reaction zone may be heated by any heating method such as high frequency plasma, induction heating, microwave heating, infrared heating, laser heating, etc. Any heating method may be used in the second reaction zone, and no further heating is required.
If the temperature is kept above the melting point of Si and below the boiling point, heating is not necessary, and conversely, cooling may be necessary.
又第１反応域と第２反応域の間に隔壁等の障害
物がある方が良い場合もある。ただ、第１反応域
で融体化かつ微細球状化したSiが生成するまで
は、炭素化合物が第１反応域に侵入しないように
しなければならない。 Further, it may be better to have an obstacle such as a partition between the first reaction zone and the second reaction zone. However, it is necessary to prevent the carbon compound from entering the first reaction zone until molten and finely spheroidized Si is produced in the first reaction zone.
さらに第１、第２反応域は非酸化性雰囲気であ
ることが望ましい。なぜならば酸素が多い場合は
SiO2が生成する可能性があるからである。 Furthermore, it is desirable that the first and second reaction zones be in a non-oxidizing atmosphere. Because if there is a lot of oxygen
This is because SiO 2 may be generated.
実施例
第１図の装置を使つて、プラズマ用ガス導入管
３からArガスを20／min導入し、陰極１と陽
極２の間で30V、400Aの条件で放電させ、プラ
ズマを発生させたのち、Si導入管５よりSiH4を
１／min導入して第１反応域４にて融体化かつ
微細球状化したSiを生成させた。この段階で採取
した球状化Siの透過電子顕微鏡による写真（６万
倍）を第３図に示す。Example Using the device shown in Figure 1, Ar gas was introduced from the plasma gas introduction tube 3 at 20/min, and discharged between the cathode 1 and anode 2 at 30V and 400A to generate plasma. , SiH 4 was introduced from the Si introduction tube 5 at 1/min to generate Si that was molten and made into fine spherules in the first reaction zone 4. Figure 3 shows a transmission electron micrograph (60,000x) of the spheroidized Si collected at this stage.
なお、この第１反応域４の直径は40mmで、温度
は2000℃以上である。 Note that the diameter of this first reaction zone 4 is 40 mm, and the temperature is 2000° C. or higher.
さらに、融体化かつ微細球状化したSiを第２反
応域に送り、炭素導入管７よりCH4を１／min
導入し、約2000℃の第２反応域６にて前記Siを炭
化しSiCを合成した。得られた球状SiCを粉末取
出口８より回収した。 Furthermore, the molten and finely spheroidized Si is sent to the second reaction zone, and CH 4 is added at 1/min from the carbon introduction pipe 7.
The Si was introduced and carbonized in the second reaction zone 6 at about 2000°C to synthesize SiC. The obtained spherical SiC was collected from the powder outlet 8.
得られたSiC粉末は第４図に示す透過電子顕微
鏡写真より判るように直径が0.1〜1.0μm程度の球
状粉末であり、主としてβ―SiCであつた。 As can be seen from the transmission electron micrograph shown in FIG. 4, the obtained SiC powder was a spherical powder with a diameter of about 0.1 to 1.0 μm, and was mainly β-SiC.
第１図は直流プラズマ利用の球状SiC粉末製造
装置の略図、第２図は外部電気炉利用の球状SiC
粉末装置の略図である。第３図は球状Si、第４図
は球状SiC粉末の粒子構造を示す透過電子顕微鏡
写真図である。
１…陰極、２…陽極、３…プラズマ用ガス導入
管、４…第１反応域、５…Si導入管、６…第２反
応域、７…炭素導入管、８…粉末取出口、９…外
部電気炉。
Figure 1 is a schematic diagram of spherical SiC powder production equipment using DC plasma, and Figure 2 is a schematic diagram of spherical SiC powder production equipment using an external electric furnace.
1 is a schematic diagram of a powder apparatus. FIG. 3 is a transmission electron micrograph showing the particle structure of spherical Si powder, and FIG. 4 is a transmission electron micrograph showing the particle structure of spherical SiC powder. DESCRIPTION OF SYMBOLS 1... Cathode, 2... Anode, 3... Gas introduction tube for plasma, 4... First reaction zone, 5... Si introduction tube, 6... Second reaction zone, 7... Carbon introduction tube, 8... Powder outlet, 9... External electric furnace.
Claims (1)
化合物を導入して、融体化かつ球状化したSiを生
成させ、この球状化SiをSiの融点以上沸点以下の
第２反応域で炭素化合物と反応させることを特徴
とする球状SiC粉末の製造法。1 Si that does not contain C in the first reaction zone above the melting point of Si
Production of spherical SiC powder characterized by introducing a compound to generate molten and spheroidized Si, and reacting the spheroidized Si with a carbon compound in a second reaction zone above the melting point of Si and below the boiling point. Law.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP58185188A JPS6077114A (en) | 1983-10-05 | 1983-10-05 | Production of spherical sic powder |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP58185188A JPS6077114A (en) | 1983-10-05 | 1983-10-05 | Production of spherical sic powder |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS6077114A JPS6077114A (en) | 1985-05-01 |
| JPS6351966B2 true JPS6351966B2 (en) | 1988-10-17 |
Family
ID=16166387
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP58185188A Granted JPS6077114A (en) | 1983-10-05 | 1983-10-05 | Production of spherical sic powder |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS6077114A (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE3650539T2 (en) * | 1985-04-04 | 1996-10-31 | Nippon Steel Corp | Process for producing silicon carbide particles and a silicon carbide sintered body |
| CN103833035B (en) * | 2014-03-06 | 2017-01-11 | 台州市一能科技有限公司 | Preparation method of silicon carbide |
-
1983
- 1983-10-05 JP JP58185188A patent/JPS6077114A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS6077114A (en) | 1985-05-01 |
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