JPH02280826A - Synthesis of diamond - Google Patents

Synthesis of diamond

Info

Publication number
JPH02280826A
JPH02280826A JP10364089A JP10364089A JPH02280826A JP H02280826 A JPH02280826 A JP H02280826A JP 10364089 A JP10364089 A JP 10364089A JP 10364089 A JP10364089 A JP 10364089A JP H02280826 A JPH02280826 A JP H02280826A
Authority
JP
Japan
Prior art keywords
diamond
seed crystal
crystal
pressure
strength
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.)
Pending
Application number
JP10364089A
Other languages
Japanese (ja)
Inventor
Manabu Miyamoto
学 宮本
Kazumitsu Tanaka
一光 田中
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Kobe Steel Ltd
Original Assignee
Kobe Steel Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Kobe Steel Ltd filed Critical Kobe Steel Ltd
Priority to JP10364089A priority Critical patent/JPH02280826A/en
Publication of JPH02280826A publication Critical patent/JPH02280826A/en
Pending legal-status Critical Current

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  • Crystals, And After-Treatments Of Crystals (AREA)
  • Carbon And Carbon Compounds (AREA)

Abstract

PURPOSE:To obtain a diamond single crystal excellent in strength by embedding a diamond seed crystal into an inert pressure medium and bringing a catalyst metal into contact with one of the faces. CONSTITUTION:When a diamond is synthetically manufactured at a high temp. and pressure using a diamond seed crystal, this seed crystal is embedded into an inert pressure medium such as salt, BN, talc, etc., with one crystal face exposed. A catalyst metal such as platinum, tantalum, etc., is brought into contact with this crystal face under pressure. This keeps carbonaceous substances from being supplied to the faces enclosed by the pressure medium and the diamond grows on the exposed face alone into a granular form, being excellent in strength.

Description

【発明の詳細な説明】 [産業上の利用分野] 本発明はダイヤモンド種結晶を用いて高温高圧下でダイ
ヤモンドを合成する方法に関し、殊に研削や切断の為に
用いられる工具用砥粒や切削工具用刃先等の材料として
有用な高強度且つ大粒のダイヤモンド単結晶を合成する
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 of synthesizing diamond under high temperature and pressure using diamond seed crystals, and in particular, to a method for synthesizing diamond under high temperature and pressure using diamond seed crystals. The present invention relates to a method for synthesizing high-strength, large-grain diamond single crystals that are useful as materials for tool cutting edges and the like.

[従来の技術] ダイヤモンドは高硬度であることを利用して古くから切
削工具用途を中心に広く利用されている。ダイヤモンド
の合成法としては、最近、気体状炭化水素を炭素原料と
して低圧条件下で行なう気相合成法が開発されているが
、この方法で合成されるダイヤモンドは粒径の小さいも
のしか得られず、ダイヤモンドを大粒の単結晶として合
成したいとぎには、従来の高温・高圧法を採用すべきで
あると考えられている。
[Prior Art] Due to its high hardness, diamond has been widely used for cutting tools since ancient times. As a method for synthesizing diamonds, a gas-phase synthesis method has recently been developed in which gaseous hydrocarbons are used as carbon raw materials under low pressure conditions, but diamonds synthesized by this method can only be obtained with small particle sizes. It is believed that the conventional high temperature and high pressure method should be used to synthesize diamond as a large single crystal.

大粒のダイヤモンド単結晶を目標とする合成方法は種々
知られているが、その代表例としてはバーバード・エム
・ストロング()1.M、strong)がJ 、Ph
ys、Chem、75. (1971) 1833に発
表したいわゆる温度差法を挙げることができる。
Various synthesis methods are known that aim to produce large diamond single crystals, and a representative example is the one described by Barbard M. Strong () 1. M, strong) is J, Ph
ys, Chem, 75. (1971) The so-called temperature difference method published in 1833 can be mentioned.

この方法は、ある方法で得られたダイヤモンドを原料と
しこれを更に大粒化する技術に関するものであって、な
んらかの方法によって製造された合成ダイヤモンドを炭
素源として高温側に配置すると共に低温側には金属触媒
を前記炭素源に接触する様に配置し、更に金属触媒の最
も低温となる部分にダイヤモンド種結晶を配置しておき
、最高温部と最低温部の温度差を約50℃に保ち、この
温度差によって炭素源が金属触媒中を拡散しつつ前記種
結晶上にダイヤモンドとして晶出し大粒ダイヤモンド単
結晶として成長させるものである。
This method uses diamond obtained by a certain method as a raw material and uses it as a raw material to further enlarge the diamond. Synthetic diamond produced by some method is placed on the high temperature side as a carbon source, and metal is placed on the low temperature side. The catalyst is placed in contact with the carbon source, and a diamond seed crystal is placed in the lowest temperature part of the metal catalyst, and the temperature difference between the highest temperature part and the lowest temperature part is maintained at about 50°C. Due to the temperature difference, the carbon source is diffused in the metal catalyst, crystallized as diamond on the seed crystal, and grown as a large diamond single crystal.

しかしながら、この方法では大粒ダイヤモンド単結晶を
得るのに長時間を要するという欠点があり、例えば1m
mの大きさまで成長させるのに2〜5時間もの長時間が
必要であった。
However, this method has the disadvantage that it takes a long time to obtain large diamond single crystals;
It took a long time of 2 to 5 hours to grow to a size of m.

一方比較的短時間にダイヤモンド(但し後述の如く小粒
径ダイヤモンド)を合成する方法としては薄膜合成法が
知られており、上記結晶成長技術よりも古く、例えば特
公昭37−4407号に開示された技術がある。この方
法は上記結晶成長技術と同じ<H,M、ストロングによ
るものであり、周期律表第■族(鉄族、白金族)に属す
る元素若しくはクロム、タンタル、マンガン等の元素或
はこれらの元素を含む合金を触媒とし、該触媒と炭素物
質(黒鉛)とを共存させた状態にして両者の共晶温度以
上の温度で且つダイヤモンド−黒鉛平衡線以上の圧力(
ダイヤモンドの熱力学的に安定な条件)下に保持して合
成するものである。
On the other hand, a thin film synthesis method is known as a method for synthesizing diamond (small-diameter diamond as described below) in a relatively short period of time, and is older than the above-mentioned crystal growth technique, for example, as disclosed in Japanese Patent Publication No. 37-4407. There is a technology that This method uses the same <H, M, Strong method as the crystal growth technique described above, and uses elements belonging to Group Ⅰ of the periodic table (iron group, platinum group), or elements such as chromium, tantalum, and manganese, or these elements. using an alloy containing carbon as a catalyst, the catalyst and a carbon material (graphite) coexisting at a temperature higher than the eutectic temperature of both, and a pressure higher than the diamond-graphite equilibrium line (
It is synthesized under conditions in which diamond is thermodynamically stable.

この様な構成を採用することによって、30分以下とい
う短時間で高強度のダイヤモンドを合成することに成功
しているが、当該方法は元々ダイヤモンド粉末を得る目
的で行なわれるものであり、0.5mm以上の大粒ダイ
ヤモンド単結晶を得ることはほとんど不可能である。そ
こでこの方法を応用することによって大粒のダイヤモン
ドを比較的早く合成する試みとして、例えば特公昭55
−11605号や特開昭59−203717号等に示す
技術が提案されている。これらの技術はダイヤモンド種
結晶を用い、この種結晶上にダイヤモンドを成長させる
ことによって、大粒のダイヤモンド単結晶を合成しよう
とするものである。尚ダイヤモンド種結晶を用いる合成
方法ではその圧力はダイヤモンドが自発核を形成し得る
最低の圧力を超えない圧力(特開昭59−203717
号)や、黒鉛−ダイヤモンド平衡線付近(2キロバ一ル
以内)の圧力(特公昭55−11605号)等に設定さ
れるのが一般的である。これは自発核を生成し得る最低
の圧力以上の圧力では、ダイヤモンド車種晶以外の部分
で核生成が頻繁に起こり、大粒のダイヤモンド単結晶が
得られないと考えられていた為である。
By employing such a configuration, we have succeeded in synthesizing high-strength diamond in a short time of 30 minutes or less, but this method was originally carried out for the purpose of obtaining diamond powder, and the 0. It is almost impossible to obtain large diamond single crystals of 5 mm or more. Therefore, as an attempt to synthesize large diamonds relatively quickly by applying this method, for example,
Techniques such as those shown in No.-11605 and Japanese Unexamined Patent Publication No. 59-203717 have been proposed. These techniques attempt to synthesize large diamond single crystals by using a diamond seed crystal and growing diamond on this seed crystal. In addition, in the synthesis method using a diamond seed crystal, the pressure is a pressure that does not exceed the lowest pressure at which diamond can form spontaneous nuclei (Japanese Patent Application Laid-Open No. 59-203717
It is generally set at a pressure near the graphite-diamond equilibrium line (within 2 kilobars) (Japanese Patent Publication No. 11605/1983). This is because it was thought that if the pressure was higher than the lowest pressure at which spontaneous nucleation could occur, nucleation would occur frequently in areas other than diamond crystals, making it impossible to obtain large diamond single crystals.

[発明が解決しようとする課題] しかしなから上記特公昭55−11605号に開示され
た技術では、ダイヤモンド種結晶を炭素物質(黒鉛)中
に埋人配胃して合成するものであるため、高強度のもの
が得られないという欠点もあった。これはダイヤモンド
種結晶とそれから成長したダイヤモンドの境界は、触媒
をとり込んだり、欠陥が発生したりしやすく、割れの起
点になりやすく、従ってダイヤモンド種結晶を包み込ん
だ形で成長したダイヤモンドは強度的に劣るという理由
によるものと思われる。尚ダイヤモンド種結晶を用いて
合成する方法としては例えば特開昭61−68395号
に開示された技術も提案されているか、この技術におい
ても溶媒金属板または非ダイヤモンド炭素板のいずれか
に多数の凹孔を形成し、この凹孔にダイヤモンド種結晶
を挿入して合成するものであり、上記技術と同様強度的
に劣ったダイヤモンド粒子しか得られない。
[Problems to be Solved by the Invention] However, in the technique disclosed in the above-mentioned Japanese Patent Publication No. 55-11605, diamond seed crystals are synthesized by burying them in carbon material (graphite). Another disadvantage was that high strength could not be obtained. This is because the boundary between a diamond seed crystal and the diamond grown from it is likely to take in catalyst or generate defects, making it a likely starting point for cracks. This seems to be due to the fact that it is inferior to As a method for synthesis using diamond seed crystals, for example, the technique disclosed in JP-A No. 61-68395 has also been proposed, and this technique also involves forming a large number of depressions in either a solvent metal plate or a non-diamond carbon plate. Synthesis is performed by forming a hole and inserting a diamond seed crystal into the hole, and as with the above technique, only diamond particles with inferior strength can be obtained.

本発明は上述した技術的課題を解決する為になされたも
のであって、本発明の目的は、ダイヤモンド種結晶を用
いる合成方法によっても、高強度のダイヤモンド単結晶
を得ようとするものである。
The present invention has been made to solve the above-mentioned technical problems, and an object of the present invention is to obtain a high-strength diamond single crystal also by a synthesis method using a diamond seed crystal. .

[課題を解決する為の手段〕 上記の目的を達成し得た本発明方法とは、金属触媒、炭
素物質およびダイヤモンド種結晶を用いて高温高圧下で
ダイヤモンドを合成する方法において、ダイヤモンド種
結晶を、その一面だけを残して圧力媒体中に埋め込み、
上記一面に触媒金属を接触させた状態でダイヤモンドを
合成する点に要旨を有するものである。
[Means for Solving the Problems] The method of the present invention that achieves the above object is a method of synthesizing diamond under high temperature and high pressure using a metal catalyst, a carbon material, and a diamond seed crystal. , embedded in a pressure medium leaving only one side of it,
The gist of this method is that diamond is synthesized with a catalyst metal in contact with the above-mentioned surface.

[作用] 本発明は上述の如く構成されるが、要は高温・高圧下で
ダイヤモンド種結晶上にダイヤモンド単結晶を成長させ
る方法を基本とし、ダイヤモンドの成長環境を適切に制
御すれば従来法よりも高強度で大粒のダイヤモンド単結
晶が短時間で成長することを見出したことに基づくもの
である。
[Function] The present invention is constructed as described above, but is basically based on a method of growing a diamond single crystal on a diamond seed crystal under high temperature and high pressure. This method is based on the discovery that a large diamond single crystal with high strength can be grown in a short period of time.

これまでのダイヤモンド合成方法では、ダイヤモンド種
結晶を炭素物質または金属触媒に埋め込んだ形態で合成
されるものであり、この様な状態で合成されたダイヤモ
ンドでは十分な強度が得られない点は既に指摘した通り
である。こうした不都合を解消するという観点から本発
明者らが検討したところ、ダイヤモンド種結晶の一面だ
けを残して不活性圧力媒体に該結晶を埋め込み、上記一
面に触媒金属を接触させた状態でダイヤモンドを合成す
る様な構成を採用すれば、強度の優れたダイヤモンド単
結晶が得られることが分かった。即ち、該構成を採用す
れば、圧力媒体に覆われた面には炭素物質が供給されず
、残った一面のみからダイヤモンドが成長するので、成
長したダイヤモンドは単結晶を包み込んだ形態ではなく
、ダイヤモンド種結晶と成長したダイヤモンドは容易に
分離でき、成長ダイヤモンド自体は粒状をしており、強
度的に優れたものとなる。これに対し、従来の方法では
ダイヤモンド種結晶を金属触媒や炭素物質等に埋め込ん
だ状態で合成するのでダイヤモンドは種結晶を包み込ん
だ形で成長し、この様な形態のダイヤモンドは上述の理
由から強度が低下する。
Conventional diamond synthesis methods involve embedding diamond seed crystals in carbon materials or metal catalysts, and it has already been pointed out that diamonds synthesized in this state do not have sufficient strength. That's exactly what I did. From the viewpoint of resolving these inconveniences, the present inventors investigated and found that the diamond seed crystal was embedded in an inert pressure medium leaving only one side of the crystal, and diamond was synthesized with the catalyst metal in contact with the one side. It was found that by adopting such a structure, a diamond single crystal with excellent strength could be obtained. In other words, if this configuration is adopted, carbon material will not be supplied to the surface covered by the pressure medium, and diamond will grow from only the remaining surface, so the grown diamond will not be in the form of enveloping a single crystal, but will be in the form of a diamond. The seed crystal and the grown diamond can be easily separated, and the grown diamond itself is granular and has excellent strength. On the other hand, in the conventional method, the diamond seed crystal is synthesized by embedding it in a metal catalyst, carbon material, etc., so the diamond grows in a form that envelops the seed crystal. decreases.

本発明で用いる圧力媒体の素材としては、ダイヤモンド
合成雰囲気に対して不活性であるとともに金属触媒とも
反応しないことが必要であり、例えば食塩、BN、タル
ク等が挙げられる。
The material for the pressure medium used in the present invention must be inert to the diamond synthesis atmosphere and not react with the metal catalyst, and examples thereof include common salt, BN, talc, and the like.

尚本発明で用いる金属触媒としては炭素物質からダイヤ
モンドを合成し得るものであればよく特に限定しないが
、例えば白金、タンタル、鉄、コバルト、ニッケル、ロ
ジウム、ルテニウム、パラジウム、オスミウム、クロム
、マンガン等が挙げられ、特に鉄族金属およびそれらの
合金が好ましい。また原料となる炭素物質としては、黒
鉛、非晶質炭素、熱分解黒鉛等が挙げられる。
The metal catalyst used in the present invention is not particularly limited as long as it can synthesize diamond from carbon materials, but examples include platinum, tantalum, iron, cobalt, nickel, rhodium, ruthenium, palladium, osmium, chromium, manganese, etc. Among them, iron group metals and alloys thereof are particularly preferred. Further, examples of the carbon material used as a raw material include graphite, amorphous carbon, and pyrolytic graphite.

以下本発明を実施例によって更に詳細に説明するが、下
記実施例は本発明を限定する性質のものではなく、前・
後記の趣旨に徴して設計変更することはいずれも本発明
の技術的範囲に含まれるものである。
Hereinafter, the present invention will be explained in more detail with reference to examples, but the following examples are not intended to limit the present invention.
Any design changes for the purposes described below are included within the technical scope of the present invention.

[実施例] 約0.5mmのダイヤモンド種結晶を、一面だけ残して
BN製圧力媒体に埋設し、この上に直径10mm、厚さ
0.2mmのコバルト板を前記一面に接触する様に配置
し、更に上記コバルト板に厚さ2.5mmの黒鉛板を積
層し、約55キロバール、1400℃で30分間加熱し
てダイヤモンドを合成し、得られたダイヤモンドの性状
について調査した。
[Example] A diamond seed crystal of about 0.5 mm was buried in a BN pressure medium leaving only one surface, and a cobalt plate with a diameter of 10 mm and a thickness of 0.2 mm was placed on top of this so as to be in contact with the one surface. Further, a graphite plate with a thickness of 2.5 mm was laminated on the above cobalt plate and heated at about 55 kbar and 1400° C. for 30 minutes to synthesize diamond, and the properties of the obtained diamond were investigated.

得られたダイヤモンドは、ダイヤモンド種結晶の一面だ
けから成長したものであり、ダイヤモンド種結晶を包み
込んでいない形態であるので、酸処理によって種結晶か
ら分離できた。また大きさは1 mm程度であり、且つ
形の整ったものであった。
The obtained diamond grew from only one side of the diamond seed crystal and did not enclose the diamond seed crystal, so it could be separated from the seed crystal by acid treatment. Moreover, the size was about 1 mm and the shape was regular.

次に、黒鉛板とコバルト板の間にダイヤモンド種結晶を
配置する以外は上記と同様にしてダイヤモンドを合成し
た。このとき得られたダイヤモンドは生成ダイヤモンド
が種結晶を90%以上包み込んだものであった。
Next, diamond was synthesized in the same manner as above except that a diamond seed crystal was placed between the graphite plate and the cobalt plate. The diamond obtained at this time was one in which the generated diamond encapsulated more than 90% of the seed crystal.

上記2つの方法によって得られたダイヤモンドの強度を
プレス法によって評価したところ、第1表に示す結果が
得られた。
When the strength of the diamonds obtained by the above two methods was evaluated by a press method, the results shown in Table 1 were obtained.

[発明の効果] 以上述べた如(本発明によれば、ダイヤモンド種結晶を
用いる方法によっても、高強度のダイヤモンド単結晶が
得られた。
[Effects of the Invention] As described above (according to the present invention), a high-strength diamond single crystal was obtained also by the method using a diamond seed crystal.

Claims (1)

【特許請求の範囲】[Claims] 金属触媒、炭素物質およびダイヤモンド種結晶を用いて
高温高圧下でダイヤモンドを合成する方法において、ダ
イヤモンド種結晶を、その一面だけを残して不活性圧力
媒体に埋め込み、上記一面に触媒金属を接触させた状態
でダイヤモンドを合成することを特徴とするダイヤモン
ドの合成方法。
In a method of synthesizing diamond under high temperature and pressure using a metal catalyst, a carbon material, and a diamond seed crystal, the diamond seed crystal is embedded in an inert pressure medium leaving only one side of the diamond seed crystal, and the catalyst metal is brought into contact with the one side. A diamond synthesis method characterized by synthesizing diamonds in a state.
JP10364089A 1989-04-24 1989-04-24 Synthesis of diamond Pending JPH02280826A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP10364089A JPH02280826A (en) 1989-04-24 1989-04-24 Synthesis of diamond

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP10364089A JPH02280826A (en) 1989-04-24 1989-04-24 Synthesis of diamond

Publications (1)

Publication Number Publication Date
JPH02280826A true JPH02280826A (en) 1990-11-16

Family

ID=14359368

Family Applications (1)

Application Number Title Priority Date Filing Date
JP10364089A Pending JPH02280826A (en) 1989-04-24 1989-04-24 Synthesis of diamond

Country Status (1)

Country Link
JP (1) JPH02280826A (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20210016363A (en) * 2018-05-31 2021-02-15 세키스이가가쿠 고교가부시키가이샤 Heat radiation composition, heat radiation member, and filler assembly for heat radiation member

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20210016363A (en) * 2018-05-31 2021-02-15 세키스이가가쿠 고교가부시키가이샤 Heat radiation composition, heat radiation member, and filler assembly for heat radiation member
JPWO2019230969A1 (en) * 2018-05-31 2021-08-05 積水化学工業株式会社 Heat dissipation composition, heat dissipation member, and filler assembly for heat dissipation member
US12384950B2 (en) 2018-05-31 2025-08-12 Sekisui Chemical Co., Ltd. Heat-dissipating composition, heat-dissipating member, and filler aggregate for heat-dissipating member

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