JPS63170207A - Production of high-purity silicon carbide powder - Google Patents
Production of high-purity silicon carbide powderInfo
- Publication number
- JPS63170207A JPS63170207A JP62000601A JP60187A JPS63170207A JP S63170207 A JPS63170207 A JP S63170207A JP 62000601 A JP62000601 A JP 62000601A JP 60187 A JP60187 A JP 60187A JP S63170207 A JPS63170207 A JP S63170207A
- Authority
- JP
- Japan
- Prior art keywords
- silicon carbide
- carbon
- silica
- hydrogen chloride
- carbide powder
- 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 description 68
- 238000004519 manufacturing process Methods 0.000 title claims description 23
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 65
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 36
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 36
- 239000000377 silicon dioxide Substances 0.000 claims abstract description 29
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910000041 hydrogen chloride Inorganic materials 0.000 claims abstract description 12
- IXCSERBJSXMMFS-UHFFFAOYSA-N hydrogen chloride Substances Cl.Cl IXCSERBJSXMMFS-UHFFFAOYSA-N 0.000 claims abstract description 12
- 239000000741 silica gel Substances 0.000 claims abstract description 7
- 229910002027 silica gel Inorganic materials 0.000 claims abstract description 7
- 239000006229 carbon black Substances 0.000 claims abstract description 6
- 230000001590 oxidative effect Effects 0.000 claims abstract description 6
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 59
- 239000003575 carbonaceous material Substances 0.000 claims description 6
- 239000007858 starting material Substances 0.000 claims description 4
- 239000011148 porous material Substances 0.000 claims description 2
- 239000012535 impurity Substances 0.000 abstract description 13
- 239000000203 mixture Substances 0.000 abstract description 4
- 238000010438 heat treatment Methods 0.000 abstract description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 20
- 239000002994 raw material Substances 0.000 description 19
- 238000000034 method Methods 0.000 description 16
- 239000002184 metal Substances 0.000 description 11
- 229910052751 metal Inorganic materials 0.000 description 11
- 229910052742 iron Inorganic materials 0.000 description 10
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 9
- 229910052802 copper Inorganic materials 0.000 description 9
- 239000010949 copper Substances 0.000 description 9
- 238000006243 chemical reaction Methods 0.000 description 8
- 238000003786 synthesis reaction Methods 0.000 description 7
- 238000004458 analytical method Methods 0.000 description 6
- 238000006722 reduction reaction Methods 0.000 description 6
- 239000004065 semiconductor Substances 0.000 description 6
- 239000000126 substance Substances 0.000 description 6
- 238000002441 X-ray diffraction Methods 0.000 description 5
- 238000004140 cleaning Methods 0.000 description 5
- 230000015572 biosynthetic process Effects 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 150000007522 mineralic acids Chemical class 0.000 description 4
- 229910052710 silicon Inorganic materials 0.000 description 4
- 239000010703 silicon Substances 0.000 description 4
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 description 3
- 239000007795 chemical reaction product Substances 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 238000011109 contamination Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 229910000077 silane Inorganic materials 0.000 description 3
- 238000000815 Acheson method Methods 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 2
- 230000002411 adverse Effects 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000011345 viscous material Substances 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
- 239000003082 abrasive agent Substances 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- 238000003763 carbonization Methods 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 238000010924 continuous production Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 125000005843 halogen group Chemical group 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 239000011812 mixed powder Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 239000005011 phenolic resin Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 239000011780 sodium chloride Substances 0.000 description 1
Abstract
Description
【発明の詳細な説明】 〔産業上の利用分野〕 本発明は、高純度炭化けい素粉末の製造方法に関する。[Detailed description of the invention] [Industrial application field] The present invention relates to a method for producing high purity silicon carbide powder.
本発明に係る炭化けい素粉末は、半４体製造用治具等金
属不純物が少ないことが要求される材料の原料として有
用である。The silicon carbide powder according to the present invention is useful as a raw material for materials that require a small amount of metal impurities, such as jigs for manufacturing half-quarts.
炭化けい素の主な製造方法としては、
（１１金属シリコンと炭素を高温で直接反応させる方法
。すなわち、Ｓｉ＋Ｃ−４ＳｉＣなる反応により、炭化
けい素を製造する方法。The main methods for producing silicon carbide include (11) a method in which metal silicon and carbon are directly reacted at high temperatures; that is, a method in which silicon carbide is produced by a reaction of Si+C-4SiC;
（２１Ｒｎ Ｓ ｉ Ｘ ａ□ （ここにＲは水素原子
またはアルキル基、Ｘはハロゲン原子、ｎ＝１〜４）で
示されるシランまたはシランと炭化水素化合物の混合物
を高温で熱分解させる方法。(21Rn S i X a□ (wherein R is a hydrogen atom or an alkyl group, X is a halogen atom, n = 1 to 4) A method of thermally decomposing a silane or a mixture of a silane and a hydrocarbon compound at a high temperature.
（３） シリカ還元法。すなわち、
ＳｉＯ□＋３Ｃ−ＳｉＣ＋２ＣＯなる反応により、炭化
けい素を製造する方法。処理温度によってα型炭化けい
素、β型炭化けい素が出来る。特に、高温型のα型炭化
けい素の製造方法は、一般にアチソン法と呼ばれ、研削
材用からいわゆるファインセラミックス用の原料まで広
く本方法で製造されている。(3) Silica reduction method. That is, a method for producing silicon carbide through the reaction SiO□+3C-SiC+2CO. Depending on the treatment temperature, α-type silicon carbide and β-type silicon carbide can be produced. In particular, the method for producing high-temperature α-type silicon carbide is generally called the Acheson method, and this method is used to produce a wide range of products from materials for abrasives to raw materials for so-called fine ceramics.
低温型のβ型炭化けい素は、いわゆるファインセラミッ
クス用の原料として、より微細で粒度範囲の狭い形状の
そろった炭化けい素粒子を得るため種々の方法が考案さ
れている。例えば、Ｓｉｎ、の加水分解によって得られ
る微粒子状のシリカを特徴とする特開昭５８−２０４８
１３号、シリカ・炭素・炭化けい素の混合粉末を特徴と
する特公昭５８−５０９２９号がある。また、上述の方
法はバッチ式であるが、特開昭５４−３３８９９号、特
開昭５５−４０５２７号、特開昭５８−２０７０８号、
特開昭５８−１９４７３１号、特開昭５９−３９７０９
号等で連続的にβ型炭化けい素を製造する方法が開示さ
れている。Low-temperature β-type silicon carbide is used as a raw material for so-called fine ceramics, and various methods have been devised to obtain finer silicon carbide particles with a narrower particle size range and uniform shape. For example, JP-A-58-2048, which features fine particulate silica obtained by hydrolysis of Sin.
No. 13, and Japanese Patent Publication No. 58-50929, which features a mixed powder of silica, carbon, and silicon carbide. Moreover, although the above-mentioned method is a batch method, JP-A-54-33899, JP-A-55-40527, JP-A-58-20708,
JP-A-58-194731, JP-A-59-39709
A method for continuously producing β-type silicon carbide is disclosed in No.
また、特公昭６０−４４２８０号は、得られるβ型炭化
けい素がウィスカー状であるが、シリカゲルとカーボン
ブラックを原料としている。Further, in Japanese Patent Publication No. 60-44280, the β-type silicon carbide obtained is in the form of whiskers, but silica gel and carbon black are used as raw materials.
等が知られている。etc. are known.
炭化けい素粉末の高純度化方法としては、ＨＣＩ、ＨＦ
５ＨＦ ＋ ＨＮＯ３等の無機酸による洗浄が一般に行
なわれている。Methods for highly purifying silicon carbide powder include HCI and HF.
Cleaning with an inorganic acid such as 5HF + HNO3 is commonly performed.
また、半導体製造用治具等の炭化けい素焼粘体の洗浄は
、上記の無機酸による洗浄に加え、塩素または塩化水素
によるガス洗浄が行なわれている。In addition to cleaning with the above-mentioned inorganic acid, gas cleaning with chlorine or hydrogen chloride is also used to clean silicon carbide sintered viscous bodies such as semiconductor manufacturing jigs.
半導体製造用治具等として使用される炭化けい素焼粘体
は、半導体に悪影響を与える鉄、銅等の金属不純物の含
有量が少ないことが要求される。Silicon carbide sintered viscous bodies used as semiconductor manufacturing jigs and the like are required to have a low content of metal impurities such as iron and copper that adversely affect semiconductors.
上記用途の炭化けい素焼粘体を製造するための原料は、
鉄、銅等の金属不純物の含有量が少な（、工業的に安定
して必要量を速やかに、しかも安価に供給可能であるこ
とが要求される。上述の観点から各製造方法を比較する
と、
金属シリコンを原料とする製造方法（１）は、高純度金
属シリコンが高価で、しかも金属シリコンの炭化が発熱
反応であるため反応を制御することが難しく、さらに、
合成される炭化けい素の粒子が比較的大きい。微細な粉
体を得るためには、粉砕を行なう必要があり、金属不純
物の汚染を受ける。The raw materials for producing the silicon carbide sintered viscous material for the above uses are:
It is required that the content of metal impurities such as iron and copper is small (and that the required amount can be supplied industrially stably and quickly and at low cost.Comparing each manufacturing method from the above point of view, In the production method (1) using metallic silicon as a raw material, high-purity metallic silicon is expensive, and carbonization of metallic silicon is an exothermic reaction, so it is difficult to control the reaction.
The synthesized silicon carbide particles are relatively large. In order to obtain fine powder, it is necessary to perform pulverization, which is subject to contamination with metal impurities.
金属不純物を除去するためには、前述の無機酸による洗
浄が必要となり更に高価なものになってしまう。In order to remove metal impurities, cleaning with the above-mentioned inorganic acid is required, which further increases the cost.
シランを原料とする製造方法（２）は、高純度の炭化け
い素微粒子が得られる。しかし、使用する原料ガスが極
めて高価であり、反応の収率も低い。Production method (2) using silane as a raw material yields highly pure silicon carbide fine particles. However, the raw material gas used is extremely expensive and the yield of the reaction is also low.
本製造方法は、純度の点では優れているが、工業的に必
要量を安定してしかも安価に供給することは困難である
。Although this production method is excellent in terms of purity, it is difficult to supply the required amount industrially stably and at low cost.
シリカを原料とする製造方法（３）は、原料面では他の
２方法に比べ安価にできるという点で有利である。The production method (3) using silica as a raw material is advantageous in that it can be produced at a lower cost than the other two methods in terms of raw materials.
アチソン法によって製造されるα型炭化けい素は、塊状
であり、製造方法（１）と同様に粉砕を行なう必要があ
る。金属不純物の汚染量は、製造方法（１）とは比べも
のにならない程大きく、前述の無機酸による洗浄を数回
行なう等多大な労力を費やしても不純物を完全に除去す
ることは極めて困難である。The α-type silicon carbide produced by the Acheson method is in the form of lumps and needs to be pulverized in the same manner as in production method (1). The amount of metal impurity contamination is incomparably greater than in production method (1), and it is extremely difficult to completely remove the impurities even if a great deal of effort is spent, such as cleaning with the aforementioned inorganic acid several times. .
低温型のβ型炭化けい素の製造に関して、特開昭５８−
２０４８１３号では、原料として使用するシリカの不純
物濃度は極めて低いが、合成時に汚染を受けて原料のシ
リカの純度を維持することは出来ていない。Regarding the production of low-temperature β-type silicon carbide, JP-A-58-
In No. 204813, the impurity concentration of the silica used as a raw material is extremely low, but the purity of the raw silica cannot be maintained due to contamination during synthesis.
特公昭５Ｂ−５０９２９号においては、合成された炭化
けい素の純度に関しては論述されておらず、発明の目的
が本発明の目的とは異なることは明らかである。Japanese Patent Publication No. 5B-50929 does not discuss the purity of synthesized silicon carbide, and it is clear that the purpose of the invention is different from the purpose of the present invention.
特開昭５４−３３８９９号、特開昭５５−４０５２７号
、特開昭５８−２０７０８号、特開昭５８−１９４７３
１号、特開昭５９−３９７０９号は、β型炭化けい素の
連続的な製造方法に関するもので、やはり合成された炭
化けい素の純度に関しては論述されていない。また、合
成された炭化けい素中には、未反応のシリカ分が％単位
で含まれ、該シリカを除去するためにＩＰ処理が必要で
ある。JP-A-54-33899, JP-A-55-40527, JP-A-58-20708, JP-A-58-19473
No. 1, JP-A No. 59-39709, relates to a continuous production method of β-type silicon carbide, and also does not discuss the purity of the synthesized silicon carbide. In addition, the synthesized silicon carbide contains unreacted silica in units of %, and IP treatment is required to remove the silica.
特公昭６０−４４２８０号においては、β型炭化けい素
ウィスカを得るという目的のために半導体に悪影響を与
える鉄、ニッケル、コバルトおよび塩化ナトリウムを加
えており、半導体製造用治具等として使用される炭化け
い素焼粘体の原料としては不適である。In Japanese Patent Publication No. 60-44280, iron, nickel, cobalt and sodium chloride, which have an adverse effect on semiconductors, are added for the purpose of obtaining β-type silicon carbide whiskers, which are used as jigs for semiconductor manufacturing. It is unsuitable as a raw material for silicon carbide sintered viscous material.
本発明の目的は、上述の問題点を解決するため、シリカ
還元法を改良することによって鉄、銅等の金属不純物の
含有量を少なく、工業的に安定して必要量を速やかに、
しかも安価に供給可能な高純度炭化けい素粉末の製造方
法を提供することにある。The purpose of the present invention is to solve the above-mentioned problems by improving the silica reduction method to reduce the content of metal impurities such as iron and copper, and to quickly and stably reduce the amount of metal impurities such as iron and copper.
Moreover, it is an object of the present invention to provide a method for producing high-purity silicon carbide powder that can be supplied at low cost.
すなわち、本発明は、シリカと炭素を出発原料として炭
化けい素を製造する方法において、該出発原料を塩化水
素を含む非酸化性雰囲気中１５００℃以上で合成し、炭
化けい素を得ることを特徴とする。さらに、本発明に使
用するシリカとしては、シリカゲルが、炭素としてはカ
ーボンブランクおよび／または加熱により炭素に変化す
る炭素質物質が好ましく、該シリカゲルの表面及び微細
な空孔中にカーボンブランクおよび／または加熱により
炭素に変化する炭素質物質を含浸させることが好ましい
。That is, the present invention is a method for producing silicon carbide using silica and carbon as starting materials, characterized in that the starting materials are synthesized at 1500° C. or higher in a non-oxidizing atmosphere containing hydrogen chloride to obtain silicon carbide. shall be. Further, the silica used in the present invention is preferably silica gel, and the carbon is preferably a carbon blank and/or a carbonaceous material that changes into carbon by heating. It is preferable to impregnate the material with a carbonaceous material that changes into carbon when heated.
ところで本発明において、塩化水素の濃度は３ｖｏ１％
〜１０ｖｏ１％であることが好ましい。By the way, in the present invention, the concentration of hydrogen chloride is 3 vol.
It is preferable that it is 10vol%.
一般的なシリカ還元法は、シリカと炭素を混合した原料
を非酸化性雰囲気で加熱することにより炭化けい素を合
成する。In a typical silica reduction method, silicon carbide is synthesized by heating a raw material mixture of silica and carbon in a non-oxidizing atmosphere.
本発明は、上記の炭化けい素合成時に塩化水素を添加す
ることによって、原料であるシリカと炭素中に含まれる
鉄、銅等の金属不純物を塩化物として揮散させることに
より高純度の炭化けい素を得ることができるという知見
に基づいてなされたものである。The present invention is capable of producing high-purity silicon carbide by adding hydrogen chloride during the synthesis of silicon carbide and volatilizing metal impurities such as iron and copper contained in the raw material silica and carbon as chloride. This was done based on the knowledge that it is possible to obtain
炭化けい素合成温度は、１５００℃以上であれば良＜１
５００℃〜２０５０℃の温度範囲では、β型炭化けい素
が、２０５０℃以上の温度範囲では、α型炭化けい素が
合成される。Silicon carbide synthesis temperature should be 1500℃ or higher <1
In the temperature range of 500°C to 2050°C, β-type silicon carbide is synthesized, and in the temperature range of 2050°C or higher, α-type silicon carbide is synthesized.
また、１５００℃以下の温度では炭化けい素の収率が極
端に悪くなるので好ましくない。Furthermore, temperatures below 1500° C. are not preferred because the yield of silicon carbide becomes extremely poor.
シリカゲルの表面及び微細な空孔中にカーボンブラック
および／または加熱により炭素に変化する炭素質物質を
含浸したものを原料とした場合、シリカ還元反応が極め
て効率良く行なわれるため炭化けい素合成反応後には、
未反応シリカはほとんど残らない。When the surface and fine pores of silica gel are impregnated with carbon black and/or a carbonaceous substance that converts into carbon when heated, the silica reduction reaction is extremely efficient, so after the silicon carbide synthesis reaction. teeth,
Almost no unreacted silica remains.
また、シリカと炭素の混合割合は、反応式Ｓｉｎｇ ＋
３Ｃ＝ＳｉＣ＋ ２ＣＯによってシリカ還元反応を完
結させるための理論炭素量の１．１〜２．０倍が良い。In addition, the mixing ratio of silica and carbon is determined by the reaction formula Sing +
3C=SiC+ 2CO is preferably 1.1 to 2.0 times the theoretical carbon amount for completing the silica reduction reaction.
理論炭素量の１．１倍以下では、未反応シリカが残留し
、理論炭素量の２．０倍以上加えても、単に反応後に反
応に携わらなかった炭素が大量に残るばかりで好ましく
ない。If the amount of carbon is less than 1.1 times the theoretical carbon amount, unreacted silica will remain, and if it is added more than 2.0 times the theoretical amount of carbon, a large amount of carbon that has not participated in the reaction will simply remain after the reaction, which is not preferable.
反応生成物には、余剰の炭素が幾分台まれているが、酸
化雰囲気中、５００℃〜７００℃で炭素を酸化して除去
することができる。Although the reaction product contains some excess carbon, it can be removed by oxidizing the carbon at 500°C to 700°C in an oxidizing atmosphere.
高純度の炭化けい素を得るために加える塩化水素の濃度
は、３ｖｏ１％〜１ｏｖｏ１％であることが好ましい。The concentration of hydrogen chloride added to obtain high purity silicon carbide is preferably 3vol% to 1ovo1%.
３ｖｏ１％以下では高純度化が十分でなく、１０νｏ１
％以上では合成された炭化けい素が塩化水素によって分
解してしまい炭化けい素の収率が悪くなってしまう。If it is less than 3vo1%, high purity is not sufficient, and 10νo1
% or more, the synthesized silicon carbide is decomposed by hydrogen chloride and the yield of silicon carbide becomes poor.
次に、本発明を実施例により説明する。 Next, the present invention will be explained by examples.
実施例１
シリカ微粉末５００ｇにカーボンブラック２１０ｇおよ
びフェノール樹脂４３０ｇ （炭素換算で１５０ ｇ）
を加えよく混合した。加えた炭素の量は理論炭素量の１
．２倍に相当する。尚、第１表中の倍率とは、（加えた
炭素量／理論炭素量）の値を表わす。Example 1 500 g of fine silica powder, 210 g of carbon black and 430 g of phenol resin (150 g in terms of carbon)
was added and mixed well. The amount of carbon added is 1 of the theoretical amount of carbon.
．． Equivalent to twice as much. Note that the magnification in Table 1 represents the value of (added carbon amount/theoretical carbon amount).
次に、該原料を２００℃で１０時間乾燥後、Ａｒ９５ｖ
ｏ１χ、ＨＣｌ５ｖｏｌ％の雰囲気中１６５０℃で４時
間合成反応を行なった。冷却後２２８．５ｇの反応生成
物を得た。該反応生成物を大気中６５０℃で５時間保持
しこ余剰の炭素を酸化して除去したところ１９４ｇの炭
化けい素を得た。Next, after drying the raw material at 200°C for 10 hours, Ar95v
The synthesis reaction was carried out at 1650° C. for 4 hours in an atmosphere of o1χ and HCl 5 vol%. After cooling, 228.5 g of reaction product was obtained. The reaction product was held in the atmosphere at 650° C. for 5 hours, and excess carbon was oxidized and removed, yielding 194 g of silicon carbide.
得られた炭化けい素のＸ線回折図形からβ型炭化けい素
と同定された。化学分析により未反応の遊離シリカ、鉄
、銅を定量したところ、遊離シリカは３．４％１ｔ％、
鉄は１０ｐｐ＋ｓ、銅はｔｐｐ−であった。Based on the X-ray diffraction pattern of the obtained silicon carbide, it was identified as β-type silicon carbide. When unreacted free silica, iron, and copper were quantified by chemical analysis, the free silica was 3.4%, 1t%,
Iron was 10 pp+s, copper was tpp-.
比較例１
雰囲気をＡｒ１００ｖｏｌ％とした他は、実施例１と全
く同一の方法で炭化けい素を合成した。得られた炭化け
い素はＸ線回折図形からβ型炭化けい素と同定されたが
、化学分析の結果遊離シリカは３．３ｗｔ％、鉄は５４
０ｐｐｍ、銅は１０ｐｐａ＋であった。Comparative Example 1 Silicon carbide was synthesized in exactly the same manner as in Example 1, except that the atmosphere was changed to 100 vol% Ar. The obtained silicon carbide was identified as β-type silicon carbide from the X-ray diffraction pattern, but chemical analysis showed that free silica was 3.3 wt% and iron was 54 wt%.
0 ppm, copper was 10 ppa+.
実施例２．３
シリカゲル微粉５５０ｇにフェノール樹ＪＩＩｆ１３０
０ｇ（炭素換算で４５５ ｇ）を加えよく混合した。Example 2.3 Phenol tree JIIf130 in 550g of silica gel fine powder
0 g (455 g in terms of carbon) was added and mixed well.
加えた炭素の量は理論炭素量の１．３８倍に相当する。The amount of carbon added corresponds to 1.38 times the theoretical amount of carbon.
該原料から第１表の条件で炭化けい素を合成した。得ら
れた炭化けい素はＸ線回折図形からβ型炭化けい素と同
定された。化学分析の結果は第１表の通りである。Silicon carbide was synthesized from the raw materials under the conditions shown in Table 1. The obtained silicon carbide was identified as β-type silicon carbide from the X-ray diffraction pattern. The results of chemical analysis are shown in Table 1.
比較例２．３
実施例２．３と同一の原料を使用し、第１表の条件で炭
化けい素を合成した。化学分析の結果未反応の遊離シリ
カが多く、炭化けい素の収率が極端に悪くなった。Comparative Example 2.3 Using the same raw materials as in Example 2.3, silicon carbide was synthesized under the conditions shown in Table 1. Chemical analysis revealed that there was a large amount of unreacted free silica, and the yield of silicon carbide was extremely poor.
実施例４
実施例２．３と同一の原料を使用し、３ｖｏｌ％のＨＣ
Ｉを含むＡｒ雰囲気中２２００℃で２時間合成反応を行
なった。得られた炭化けい素はＸ線回折図形からβ型炭
化けい素と同定された。化学分析の結果は第１表の通り
である。Example 4 Using the same raw materials as Example 2.3, 3 vol% HC
The synthesis reaction was carried out at 2200° C. for 2 hours in an Ar atmosphere containing I. The obtained silicon carbide was identified as β-type silicon carbide from the X-ray diffraction pattern. The results of chemical analysis are shown in Table 1.
比較例４
雰囲気をＡｒ１００ｖｏｌ％とした他は、実施例４と全
く同一の方法で炭化けい素を合成した。得られた炭化け
い素はＸ線回折図形からα型炭化けい素と同定された。Comparative Example 4 Silicon carbide was synthesized in exactly the same manner as in Example 4, except that the atmosphere was changed to 100 vol% Ar. The obtained silicon carbide was identified as α-type silicon carbide from the X-ray diffraction pattern.
化学分析の結果は第１表の通りである。The results of chemical analysis are shown in Table 1.
上述したように本発明によれば、シリカ還元法による炭
化けい素の合成において合成時に塩化水素を添加するこ
とにより、半導体製造用治具等として使用される炭化け
い素焼粘体用の原料として好適な鉄、銅等の金属不純物
の含有量が少ない高純度炭化けい素粉末を工業的に安定
して必要量を速やかに、しかも安価に供給出来た。今後
、炭化けい素の用途が広まる中で本発明の産業上の役割
は大といえる。As described above, according to the present invention, by adding hydrogen chloride during the synthesis of silicon carbide by the silica reduction method, it is possible to obtain a material suitable as a raw material for silicon carbide sintered viscous bodies used as semiconductor manufacturing jigs, etc. High-purity silicon carbide powder with a low content of metal impurities such as iron and copper could be industrially stably supplied in the required amount quickly and at low cost. It can be said that the present invention will play a major role in industry as the uses of silicon carbide expand in the future.
特許出願人 東海高熱工業株式会社
手続補正書
昭和６２年 ６月／♂日
特許庁長官 黒 １） 明 雄 殿１６事件の
表示
昭和６２年特許願第 ６０１号
２、発明の名称
３、補正をする者
事件との関係 特許出願人
トウ愈イスウネッゴウギコウヵブシキヵイシャ名称 東
海高熱工業株式会社
７、補正の内容
明細書１２ペ一ジ９行目の“β型”を「α型」と訂正す
る。Patent Applicant Tokai Konetsu Kogyo Co., Ltd. Procedural Amendment June 1986 / ♂ Date Commissioner of the Patent Office Black 1) Akio Tono Indication of Case 16 Patent Application No. 601 of 1988 2, Name of the Invention 3, Make amendments Relationship with the patent applicant's case Name: Tokai Kounetsu Kogyo Co., Ltd. 7, "β-type" in line 9 of page 12 of the amended statement of contents was changed to "α-type" correct.
Claims (1)
る方法において、該出発原料を塩化水素を含む非酸化性
雰囲気中１５００℃以上で合成し、炭化けい素を得るこ
とを特徴とする高純度炭化けい素粉末の製造方法。 ２、シリカとしてシリカゲルを用い、炭素としてカーボ
ンブラックおよび／または加熱により炭素に変化する炭
素質物質を用いて、該シリカゲルの表面及び微細な空孔
中にカーボンブラックおよび／または加熱により炭素に
変化する炭素質物質を含浸する特許請求の範囲第１項記
載の高純度炭化けい素粉末の製造方法。 ３、塩化水素の濃度が３ｖｏｌ％〜１０ｖｏｌ％である
特許請求の範囲第１項または第２項記載の高純度炭化け
い素粉末の製造方法。[Claims] 1. A method for producing silicon carbide using silica and carbon as starting materials, in which the starting materials are synthesized at 1500°C or higher in a non-oxidizing atmosphere containing hydrogen chloride to obtain silicon carbide. A method for producing high-purity silicon carbide powder, characterized by: 2. Using silica gel as the silica, using carbon black and/or a carbonaceous substance that changes to carbon when heated as the carbon, and using carbon black and/or a carbonaceous substance that changes to carbon when heated on the surface and fine pores of the silica gel. A method for producing high-purity silicon carbide powder according to claim 1, which comprises impregnating a carbonaceous material. 3. The method for producing high-purity silicon carbide powder according to claim 1 or 2, wherein the concentration of hydrogen chloride is 3 vol% to 10 vol%.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62000601A JPH062568B2 (en) | 1987-01-07 | 1987-01-07 | Method for producing high-purity silicon carbide powder |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62000601A JPH062568B2 (en) | 1987-01-07 | 1987-01-07 | Method for producing high-purity silicon carbide powder |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS63170207A true JPS63170207A (en) | 1988-07-14 |
| JPH062568B2 JPH062568B2 (en) | 1994-01-12 |
Family
ID=11478250
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62000601A Expired - Lifetime JPH062568B2 (en) | 1987-01-07 | 1987-01-07 | Method for producing high-purity silicon carbide powder |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH062568B2 (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2006256941A (en) * | 2005-03-18 | 2006-09-28 | Toda Kogyo Corp | Method for manufacturing silicon carbide powder |
| CN115087620A (en) * | 2020-01-31 | 2022-09-20 | 弗劳恩霍夫应用研究促进协会 | Method for separating impurities from silicon carbide and silicon carbide powder subjected to temperature treatment and purification treatment |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP6792412B2 (en) * | 2016-10-28 | 2020-11-25 | 太平洋セメント株式会社 | Method for manufacturing silicon carbide powder |
-
1987
- 1987-01-07 JP JP62000601A patent/JPH062568B2/en not_active Expired - Lifetime
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2006256941A (en) * | 2005-03-18 | 2006-09-28 | Toda Kogyo Corp | Method for manufacturing silicon carbide powder |
| CN115087620A (en) * | 2020-01-31 | 2022-09-20 | 弗劳恩霍夫应用研究促进协会 | Method for separating impurities from silicon carbide and silicon carbide powder subjected to temperature treatment and purification treatment |
| CN115087620B (en) * | 2020-01-31 | 2024-05-07 | 弗劳恩霍夫应用研究促进协会 | Method for separating impurities from silicon carbide and temperature-treated and purified silicon carbide powder |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH062568B2 (en) | 1994-01-12 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| JPS6112844B2 (en) | ||
| JPS5913442B2 (en) | Manufacturing method of high purity type silicon nitride | |
| JPS63170207A (en) | Production of high-purity silicon carbide powder | |
| JPS62241812A (en) | Manufacture of silicon nitride | |
| JPS6111886B2 (en) | ||
| JP2721678B2 (en) | β-silicon carbide molded body and method for producing the same | |
| US4582696A (en) | Method of making a special purity silicon nitride powder | |
| JPS5839764B2 (en) | Method for producing aluminum nitride powder | |
| JPH0553723B2 (en) | ||
| JPS5930645B2 (en) | Manufacturing method of high purity α-type silicon nitride | |
| US4795622A (en) | Method for producing silicon-imide | |
| US4914063A (en) | Process for producing organic products containing silicon, hydrogen, nitrogen, and carbon by the direct reaction between elemental silicon and organic amines | |
| JPS60195099A (en) | Production of silicon nitride whisker | |
| JPH0543210A (en) | Production of high purity phosphorus | |
| JPS6111885B2 (en) | ||
| JPS61201608A (en) | Manufacture of high purity aluminum nitride powder | |
| JPH03193617A (en) | Production of silicon carbide powder | |
| JPH0313166B2 (en) | ||
| JPS62143805A (en) | Removal of chlorine and/or fluorine from silicon nitride powder | |
| JPS62216907A (en) | Manufacture of low carbon content silicon nitride | |
| JPH0218310A (en) | Preparation of zirconium-containing ceramic powder | |
| Pugar et al. | Process for producing organic products containing silicon, hydrogen, nitrogen, and carbon by the direct reaction between elemental silicon and organic amines and products formed thereby | |
| JPH0454610B2 (en) | ||
| JPH05326B2 (en) | ||
| JPS63248798A (en) | Production of silicon carbide whisker |