JPS63274609A - Synthesis of silicon carbide particle - Google Patents
Synthesis of silicon carbide particleInfo
- Publication number
- JPS63274609A JPS63274609A JP62107822A JP10782287A JPS63274609A JP S63274609 A JPS63274609 A JP S63274609A JP 62107822 A JP62107822 A JP 62107822A JP 10782287 A JP10782287 A JP 10782287A JP S63274609 A JPS63274609 A JP S63274609A
- Authority
- JP
- Japan
- Prior art keywords
- reaction
- silicon carbide
- silane
- acetylene
- aliphatic hydrocarbon
- 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
Links
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 title claims abstract description 22
- 229910010271 silicon carbide Inorganic materials 0.000 title claims abstract description 21
- 239000002245 particle Substances 0.000 title claims abstract description 16
- 230000015572 biosynthetic process Effects 0.000 title description 2
- 238000003786 synthesis reaction Methods 0.000 title description 2
- 238000000034 method Methods 0.000 claims abstract description 15
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910000077 silane Inorganic materials 0.000 claims abstract description 13
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 claims abstract description 12
- 230000002194 synthesizing effect Effects 0.000 claims abstract description 6
- -1 methane Chemical class 0.000 claims abstract description 5
- 238000006243 chemical reaction Methods 0.000 abstract description 30
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 abstract description 17
- 239000007789 gas Substances 0.000 abstract description 13
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 abstract description 9
- 150000001338 aliphatic hydrocarbons Chemical class 0.000 abstract description 5
- KDKYADYSIPSCCQ-UHFFFAOYSA-N but-1-yne Chemical compound CCC#C KDKYADYSIPSCCQ-UHFFFAOYSA-N 0.000 abstract description 4
- 238000005245 sintering Methods 0.000 abstract description 3
- 239000004215 Carbon black (E152) Substances 0.000 abstract description 2
- 238000005260 corrosion Methods 0.000 abstract description 2
- 230000007797 corrosion Effects 0.000 abstract description 2
- 239000010419 fine particle Substances 0.000 abstract description 2
- 229930195733 hydrocarbon Natural products 0.000 abstract description 2
- 150000002430 hydrocarbons Chemical class 0.000 abstract description 2
- MWWATHDPGQKSAR-UHFFFAOYSA-N propyne Chemical compound CC#C MWWATHDPGQKSAR-UHFFFAOYSA-N 0.000 abstract description 2
- 239000007792 gaseous phase Substances 0.000 abstract 2
- 239000007787 solid Substances 0.000 abstract 2
- 238000002474 experimental method Methods 0.000 description 12
- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 description 4
- 125000001931 aliphatic group Chemical group 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 229930195734 saturated hydrocarbon Natural products 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- XNMQEEKYCVKGBD-UHFFFAOYSA-N 2-butyne Chemical compound CC#CC XNMQEEKYCVKGBD-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 229910000041 hydrogen chloride Inorganic materials 0.000 description 2
- IXCSERBJSXMMFS-UHFFFAOYSA-N hydrogen chloride Substances Cl.Cl IXCSERBJSXMMFS-UHFFFAOYSA-N 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 239000001294 propane Substances 0.000 description 2
- VXEGSRKPIUDPQT-UHFFFAOYSA-N 4-[4-(4-methoxyphenyl)piperazin-1-yl]aniline Chemical compound C1=CC(OC)=CC=C1N1CCN(C=2C=CC(N)=CC=2)CC1 VXEGSRKPIUDPQT-UHFFFAOYSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 239000012776 electronic material Substances 0.000 description 1
- 238000010574 gas phase reaction Methods 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000010297 mechanical methods and process Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 238000007348 radical reaction Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000005049 silicon tetrachloride Substances 0.000 description 1
- 239000011882 ultra-fine particle Substances 0.000 description 1
Landscapes
- Carbon And Carbon Compounds (AREA)
Abstract
Description
【発明の詳細な説明】
［産業上の利用分野］
本発明は、構造材や電子材料セラミックスとして使用さ
れる炭化珪素粒子の合成方法に関するものである。DETAILED DESCRIPTION OF THE INVENTION [Industrial Application Field] The present invention relates to a method for synthesizing silicon carbide particles used as structural materials and electronic material ceramics.
［従来技術及び発明が解決しようとする問題点］今日、
セラミックス原料において、融点が高く、硬度も硬い等
の優れた特性を有するものとして炭化珪素（ｓｉｃ）が
着目されている。しかるに従来。[Prior art and problems to be solved by the invention] Today,
BACKGROUND ART Among ceramic raw materials, silicon carbide (SIC) is attracting attention as it has excellent properties such as a high melting point and hardness. However, conventionally.
この炭化珪素は、焼結することを考慮した場合に。When this silicon carbide is considered to be sintered.
微細でしかも粒径が揃い、かつ可及的に球形であること
が好ましい、このため塊体を粉砕して形成する機械的手
法によるものではなく、化学的合成による手法が採用さ
れることになる。そしてこの場合、焼結に適するため炭
化珪素を合成するには、例えば四塩化珪素（Ｓｔ ＣＱ
４ ）とメタン、プロパン等の脂肪族飽和炭化水素と
を気相で反応させて合成することが知られているが、こ
の場合には生成物として塩化水素（ＨＣＱ）が生じ、こ
れの捕集や反応器機に対する腐食等の悪影響等の欠点が
ある。It is preferable that the particles be fine, uniform in particle size, and as spherical as possible.For this reason, a chemical synthesis method is used instead of a mechanical method of crushing a lump to form it. . And in this case, to synthesize silicon carbide because it is suitable for sintering, silicon tetrachloride (St CQ
4) and aliphatic saturated hydrocarbons such as methane and propane in the gas phase, but in this case hydrogen chloride (HCQ) is produced as a product, which must be collected. There are disadvantages such as adverse effects such as corrosion on reactor equipment.
そこでシラン（ＳｉＨ−）とプロパン等の脂肪族飽和炭
化水素を反応させて合成することが試みられているが、
この場合には１反応器度が約１４００〜１５００度と高
温にする必要がある詐りでなく、生成される炭化珪素は
中空状態となってしまうという問題がある。Therefore, attempts have been made to synthesize silane (SiH-) by reacting it with aliphatic saturated hydrocarbons such as propane.
In this case, there is a problem that one reactor temperature needs to be high, about 1400 to 1500 degrees, and the silicon carbide produced ends up being in a hollow state.
ｃ問題を解決するための手段］
本発明は、上記の如き実情に鑑みこれらの欠点を一掃す
ることができる炭化珪素粒子の合成方法を提供すること
を目的として創案されたものであって、シランとアセチ
レン系脂肪族炭化水素とを気相にて反応させて成ること
を特徴とするものである。Means for Solving Problem c] In view of the above-mentioned circumstances, the present invention was devised for the purpose of providing a method for synthesizing silicon carbide particles that can eliminate these drawbacks. It is characterized by being formed by reacting the acetylene-based aliphatic hydrocarbon with an acetylene-based aliphatic hydrocarbon in the gas phase.
そして本発明は、この方法によって、塩化水素の発生の
ない反応系でありながら、反応温度を低くでき、かつ中
空ではない稠密な微細粒子の炭化珪素を生成することが
できるようにしたものである。According to the present invention, this method allows the reaction temperature to be lowered while using a reaction system in which no hydrogen chloride is generated, and it is possible to produce silicon carbide in the form of dense, fine particles that are not hollow. .
そして本発明に用いるアセチレン系脂肪族炭化水素とし
ては、アセチレン（ＣＨ＝ＣＨ）、プロピン（ＣＨ，Ｃ
ＥＣＨ）、１−ブチン（Ｃ２ＨｓＣ：ＣＨ）、２−ブチ
ン（ＣＨ，ＣＥＣＣＨ，）、１゜３−ブタジイン（Ｃ）
（ミＣＣミＣＨ）等の低級のものを単独または混合して
使用することができるが、この場合の反応式は、例えば
炭化水素がアセチレンである場合、
Ｃ，Ｈ，＋２８ｉＨ，−＋２８ｉＣ＋５Ｈ。The acetylene aliphatic hydrocarbons used in the present invention include acetylene (CH=CH), propyne (CH,C
ECH), 1-butyne (C2HsC:CH), 2-butyne (CH,CECCH,), 1゜3-butadiyne (C)
Lower compounds such as (miCCmiCH) can be used alone or in combination. In this case, for example, when the hydrocarbon is acetylene, the reaction formula is: C, H, +28iH, -+28iC+5H.
で示されることになる。そしてその反応はラジカル反応
であると推論でき、その過程は。This will be shown as It can be inferred that the reaction is a radical reaction, and the process is.
［シラン→シランラジカル→ＳｉＣクラスター→＆Ｃ超
微粒子↑
アセチレンラジカル 」によるものと
推定される６そしてこの場合、後述するような反応温度
の低下は、メタンのような脂肪族飽和炭化水素の如くラ
ジカルへの分解温度が。[silane → silane radical → SiC cluster → &C ultrafine particles ↑ acetylene radical] 6 And in this case, the decrease in reaction temperature as described below is due to the formation of radicals such as aliphatic saturated hydrocarbons such as methane. The decomposition temperature of
メタンよりもアセチレンのほうが低温で成されることに
よるものであると推論できる。It can be inferred that this is because acetylene is formed at a lower temperature than methane.
次に、本発明が如何に有効であるかを実験例によって具
体的に説明する。Next, how effective the present invention is will be specifically explained using experimental examples.
［実験１］
本実験で用いた反応装置は第１図に示す如きものであっ
て１反応器１を水冷式円筒型ノズルフィーダー２（可動
式）と周囲のハニカム３．ハイアルミナ製反応管４によ
って構成し、シランガスはノズル側から水素ガス雰囲気
下で供給し、アセチレンガスはハニカム側から同じく水
素ガス雰囲気下で供給するという拡散混合方式により反
応させた。その場合の反応条件として、シラン供給量は
５２ＩＩＱＺ■、フィーダハニカムでの出口流速は７０
ａＩｌ／Ｓと一定にした。そして生成粒子は吸引口５か
ら吸引し、フィルタ捕集をした。捕集された粒子はＣｕ
−にα線を使用した粉末Ｘ線回折を行い、捕集粒子中の
炭化珪素、珪素、炭素の含有率を各々の強度比から求め
、その結果を表１の実験１において１反応温度を変化さ
せたもの、およびモル比を変化させたものとしてし４の
項に示す。[Experiment 1] The reaction apparatus used in this experiment was as shown in FIG. The reactor was composed of a reaction tube 4 made of high alumina, and the reaction was carried out by a diffusion mixing method in which silane gas was supplied from the nozzle side under a hydrogen gas atmosphere, and acetylene gas was supplied from the honeycomb side under a hydrogen gas atmosphere. In that case, the reaction conditions are that the silane supply amount is 52IIQZ■, and the outlet flow rate at the feeder honeycomb is 70
It was kept constant at aIl/S. The generated particles were then suctioned through the suction port 5 and collected by a filter. The collected particles are Cu
- Perform powder X-ray diffraction using alpha rays to determine the content of silicon carbide, silicon, and carbon in the collected particles from their respective intensity ratios, and use the results in Experiment 1 in Table 1 by changing the reaction temperature. Items with different molar ratios and those with different molar ratios are shown in Section 4.
［実験２］
実験１で用いた反応装置および反応条件をそのまま用い
１反応方式については、シランガスとアセチレンガスと
を水素ガス雰囲気下で予め混合させてからノズルより供
給する予混合方式によって反応させた。そしてその結果
を表１の実験２の１〜ｍの項に示す、これについても反
応温度による検討１モル比による検討をした。[Experiment 2] Using the same reaction apparatus and reaction conditions as used in Experiment 1, reaction method 1 involved a premixing method in which silane gas and acetylene gas were mixed in advance in a hydrogen gas atmosphere and then supplied from a nozzle. . The results are shown in sections 1 to m of Experiment 2 in Table 1. This was also investigated by reaction temperature and 1 molar ratio.
［実験３］
実験１で用いた反応装置および反応条件をそのまま用い
、かつ実験例２の予混合方式により気相反応をさせたが
、その場合に、反応ガスの吹き込み位置を、実験２の人
位置の場合よりも炉内滞留時間が１４５製程短くなるＢ
位置に移動させて反応させた。そしてその結果を表１の
実験３のＩ −ＩＩＩの項に示す。[Experiment 3] Using the same reaction apparatus and reaction conditions as used in Experiment 1, a gas phase reaction was carried out using the premixing method of Experiment Example 2. Residence time in the furnace is 145 times shorter than in the case of position B
Moved to position and reacted. The results are shown in sections I-III of Experiment 3 in Table 1.
［比較例］
実験１で用いた反応装置および反応条件をそのまま用い
、前述した予混合方式によりシランガスとメタンガス（
ＣＨ４）とを反応させ、その結果を表１の比較例のＩ〜
■の項に示す。[Comparative Example] Using the same reaction apparatus and reaction conditions as used in Experiment 1, silane gas and methane gas (
CH4) and the results are shown in Comparative Examples I~ in Table 1.
Shown in section ■.
表 １
但し：混合方式で、■は拡散方式、■は予混合方式を意
味し。Table 1 However: In the mixing method, ■ means the diffusion method and ■ means the premixing method.
ノズル位！ＩＡ、Ｂは図面のＡ位置、Ｂ位置を示す。Nozzle position! IA and B indicate positions A and B in the drawing.
これらの結果から判断して、シランガスにメタンガスを
反応させた従来の場合では１反応器度が１３００度でも
炭化珪素の生成率が２０％と低く、少なくとも１４００
度の温度が必要であったが、本発明では反応温度が１２
００度でも条件によっては１００％という高い生成率を
示しており、これによって本発明が如何に有効であるか
が判断される。Judging from these results, in the conventional case where methane gas is reacted with silane gas, the production rate of silicon carbide is as low as 20% even when the temperature of one reactor is 1300 degrees, and at least 1400 degrees
However, in the present invention, the reaction temperature is 12°C.
Even at 00 degrees Celsius, the production rate is as high as 100% depending on the conditions, and it can be judged from this how effective the present invention is.
しかも生成した炭化珪素の粒径も、可成り揃っており、
かつその形状も、Ｘ線による写真で示す如く略球形であ
って、かつメタンガスを用いた比較例の如く中空状では
なく、完全に１１密状であることがｌ１ｌＩ８１！され
る。Moreover, the particle size of the silicon carbide produced is quite uniform,
Moreover, its shape is approximately spherical as shown in the X-ray photograph, and it is not hollow like in the comparative example using methane gas, but is completely 11 dense. be done.
しかも反応条件として、ノズル位置をＡではなくＢと炉
内滞留時間が長い場合が低温（１２００度の場合）での
生成率の点からも好ましいが、さらに生成した炭化珪素
の粒径の点においてもこの場合の方が大きな径となって
いることが観測される。Furthermore, as a reaction condition, it is preferable to set the nozzle position to B instead of A and to have a long residence time in the furnace, in terms of the production rate at low temperature (1200 degrees), but it is also preferable in terms of the particle size of the silicon carbide produced. It is also observed that the diameter is larger in this case.
これは炉内滞留時間が長くなったことによって、粒子の
成長があることを意味しており、従って炉内滞留時間の
調整により粒径の調整を可成りの範囲で行うことができ
るものであると推論される。This means that particles grow due to longer residence time in the furnace, and therefore particle size can be adjusted within a considerable range by adjusting residence time in the furnace. It is inferred that
［効果］
以上要するに１本発明は叙述の如く構成されたものであ
るから、炭化珪素を合成するに、シランとアセチレン系
脂肪族炭化水素とを気相にて反応させたことにより、反
応温度を、従来のメタン等の脂肪族飽和炭化水素と反応
させて合成するものに比して低くすることができる許り
でなく、生成される炭化珪素も１球形に近く、かつ稠密
なものにできることとなり、もって焼結するための良質
な炭化珪素を容易に提供できるものである。[Effects] In summary, 1. The present invention is constructed as described above, so that when synthesizing silicon carbide, silane and acetylene aliphatic hydrocarbon are reacted in the gas phase, thereby reducing the reaction temperature. Not only can the silicon carbide be lower than that of conventional products synthesized by reacting with aliphatic saturated hydrocarbons such as methane, but the silicon carbide produced can also be close to spherical and dense. , it is possible to easily provide high quality silicon carbide for sintering.
図面は１本発明に係る炭化珪素粒子の合成方法の実施例
を示したものであって、第１図は反応装置の概略断面図
、第２図Ａ、Ｂは実験２の■、比較例■の電子顕微鏡に
より写した代用写真図である。
図中、１は反応器、２はノズルフィーダー、３はハニカ
ム、４は反応管である。The drawings show an example of the method for synthesizing silicon carbide particles according to the present invention, in which FIG. 1 is a schematic cross-sectional view of a reaction apparatus, and FIGS. 2A and B are Experiment 2 (■) and Comparative Example (■). This is a substitute photograph taken using an electron microscope. In the figure, 1 is a reactor, 2 is a nozzle feeder, 3 is a honeycomb, and 4 is a reaction tube.
Claims (1)
させて成ることを特徴とする炭化珪素粒子の合成方法。A method for synthesizing silicon carbide particles characterized by reacting silane and an acetylene aliphatic hydrocarbon in a gas phase.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62107822A JPS63274609A (en) | 1987-04-30 | 1987-04-30 | Synthesis of silicon carbide particle |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62107822A JPS63274609A (en) | 1987-04-30 | 1987-04-30 | Synthesis of silicon carbide particle |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS63274609A true JPS63274609A (en) | 1988-11-11 |
| JPH0587443B2 JPH0587443B2 (en) | 1993-12-16 |
Family
ID=14468918
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62107822A Granted JPS63274609A (en) | 1987-04-30 | 1987-04-30 | Synthesis of silicon carbide particle |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS63274609A (en) |
-
1987
- 1987-04-30 JP JP62107822A patent/JPS63274609A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0587443B2 (en) | 1993-12-16 |
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