JPS5899199A

JPS5899199A - Synthesizing method for artificial beryl single crystal by pulling method

Info

Publication number: JPS5899199A
Application number: JP19515081A
Authority: JP
Inventors: Toshiyuki Hirose; 広瀬　敏幸
Original assignee: Matsushima Kogyo KK; Seiko Epson Corp; Suwa Seikosha KK
Current assignee: Matsushima Kogyo KK; Seiko Epson Corp; Suwa Seikosha KK
Priority date: 1981-12-04
Filing date: 1981-12-04
Publication date: 1983-06-13
Also published as: JPH0224799B2

Abstract

PURPOSE:To improve quality and to increase yield markedly in synthesis of an artificial beryl single crystal by installing a simple pulling device which is so arranged as to add beryl crystal into the fused salt of raw materials, and to pull up the single crystal by rotating the same. CONSTITUTION:A beryl crystal 2 is added into the raw material produced by adding the aluminum beryllate, silicon oxide and chromium oxide exhibiting approximately the compsn. ratios of natural beryllium and other coloring agents or a fused salt prepd. by using natural beryllium powder as a raw material and adding >=1 kind among molybdic acid, V2O5, tungstic acid, etc. and heating the same. Here the crystal 2 is fixed to a shaft 1 by means of a chuck or the like and is immersed in the fused salt of 750-1,200 deg.C with a heater 5. The shaft 1 is rotated at 1-200 rpm; at the same time, a crucible 3 is rotated at the same number of revolutions in the direction reverse from that of the shaft 1, and the crystal is pulled at 0.05-0.5mm. speed in a day. The improvement in quality and yield and the reduction in cost are resulted from the mere addition of the simple pulling device.

Description

【発明の詳細な説明】本発明は溶剤を用いた人工ベリル単結晶の合成方法に関
し、溶融塩より実質なベリル単結晶を効率よく且つ経済
的に合成し育成する方法に関するものである。これまで
人工ベリルの合成方法として、水熱法、溶融塩法が知ら
れているが本発明は溶融塩法の改良に関するものでるる
。DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a method for synthesizing an artificial beryl single crystal using a solvent, and more particularly to a method for efficiently and economically synthesizing and growing a beryl single crystal that is more substantial than a molten salt. Hitherto, hydrothermal methods and molten salt methods have been known as methods for synthesizing artificial beryl, but the present invention relates to improvements in the molten salt methods.

溶融塩法は水熱法罠比較して、エネルギー、装置等大幅
に節減でき、著しく経済的である。しかしながらこの溶
融塩法においてもなお次のような問題点がある。Compared to the hydrothermal method, the molten salt method can significantly save energy, equipment, etc., and is extremely economical. However, this molten salt method still has the following problems.

１）−曲のバッチに仕込んだ原料物質に対する高純度の
ベリル生成比か低い。1) - Low production ratio of high purity beryl to the raw material charged to the song batch.

２）溶融塩中での生成は生成速度を速くすることにより
内部狭ザツ物（インクルージヨン）が発生する。2) When forming in a molten salt, internal inclusions are generated by increasing the formation rate.

６）高品位ベリルを生成するためには生成速駅をおとし
、兼期間の育成が必要でめる。・このため大型サイズの
ベリル単結晶を作るには効率が悪い。6) In order to produce high-grade beryl, it is necessary to reduce the production speed and cultivate it for a certain period.・For this reason, it is inefficient to produce large-sized beryl single crystals.

４）溶−塊法では生成が溶融液中で行なわれるため観察
が難しい。4) In the melt-bulk method, observation is difficult because the formation takes place in the melt.

本発明は上記間鴫点を解決する新しい手法でろる。ベリ
ル合成ＶＣおいて添加ベリル表面に均一な過飽和域を出
現させることにより育成させるものであり、過飽和域出
現のために伽度會徐々に下降させる。ルツボ内のパンフ
ル悴による温度差出現させる、あるいはこの２方法を合
わ４ｔたものでろるが、いづれも溶融塩中で行なうもの
である。このＪＫ着目し改曳し九本のが第１図の方法で
ある。The present invention provides a new method for solving the above-mentioned problems. In beryl synthetic VC, beryl is grown by making a uniform supersaturated region appear on the surface of the added beryl, and the degree of beryl is gradually lowered to make the supersaturated region appear. This can be done by creating a temperature difference due to the temperature difference in the crucible, or by combining 4 tons of these two methods, but both methods are carried out in molten salt. The method shown in Figure 1 is based on nine modified methods focusing on JK.

■にベリル■ｔチャック等により固定させ■ヒターによ
シフ５０℃〜１２００℃のある所定の一度に加熱された
溶融塩中に浸漬させ（９をＩＲＰＭ〜２０°口ＲＰＭの
おる所定の回転数を持って回転させる。同時に■を■と
は逆方向に■と同一回転数を持って回転させる。■Ｆ１
更に１日にα０５■〜１５箇のある所定の速度で引上げ
る。■ Beryl ■ Fix it with a chuck etc. ■ Immerse it in a heated molten salt at a temperature of 50°C to 1200°C using a heater. Hold and rotate. At the same time, rotate ■ in the opposite direction to ■ with the same number of rotations as ■. ■F1
Furthermore, it is pulled up at a predetermined speed of α05■ to 15 times per day.

この方法罠より、 ■　添加ベリル及びルツボが回転することにより、添加
ベリルの表面近ボウは原料が均一に分布される。From this method, (1) By rotating the added beryl and the crucible, the raw material is uniformly distributed near the surface of the added beryl.

■　添加ベリルは■に接続されているため添加ベリル表
面け■に熱が伝導され冷却効果１＋たらすことＫよシ溶
融塩とベリルに温度差ができ生成する。(2) Since the added beryl is connected to (2), heat is conducted to the surface of the added beryl (2), resulting in a cooling effect of 1+.There is a temperature difference between the molten salt and the beryl, and the product is formed.

このため特に高度なｍ度管理を必要としない。For this reason, particularly sophisticated degree management is not required.

■　添加ベリルを固定した■を上昇さぜることによシ、
ベリルの育成と観察ができる。■ By stirring ■ with fixed added beryl,
You can grow and observe beryl.

実施例１１、　原料物質、溶剤ならびに配合ベリル粉末　　　１０ＦＬｒ１Ｍ６Ｑ４　　　　　　　　　　　１　　５　　０
　　　ＦＭｏ０３　　　　１ｂＯｆＣｒ１０１　　　　　　ｃＬ２ｆ ′ＬＩＶ！融塩形成の瀾度条自省るつぼ内の１の材料を充填して９００℃にて１０　
Ｈｒａ　　の保持五　ベリル株加と回転ベリルを溶融塩中ｒＣ浸漬さぜベリル及びルツボ會５　
ＯＲＰＭ　　にて回転さぜ２４　Ｈｒ−保持する。Example 1 1. Raw material, solvent and blended beryl powder 10F Lr1M6Q4 1 5 0
FMo03 1bOf Cr101 cL2f 'LIV! The degree of molten salt formation was filled with the material in the crucible and heated at 900°C for 10 minutes.
Retention of Hra 5 Addition of beryl stock and rotating beryl immersed in rC in molten salt Beryl and crucible 5
Rotate at ORPM and hold for 24 hours.

歳　引上げ条件２４Ｈｒｓ　　保持後［１２ｖｍ　７日の割合で５０日
間引上げを行った。その後湯水にて醇出処理をし合成エ
メラルドを得た。After holding for 24 hours, pulling was carried out at a rate of 12 vm for 7 days for 50 days. After that, a synthetic emerald was obtained by elution treatment with hot water.

５、ｌＷＩ果及び所見０′　屈折４　　　１．５６４〜１．５６１０比重　２
．６４ｏ　インクルージヨンが少ない。5, IWI results and findings 0' Refraction 4 1.564-1.5610 Specific gravity 2
．． 64 o Few inclusions.

実施例２１、　　ｆｉ料物買溶剤ならびに配合ベリル粉末　　　　１０ｔｖ、ｏ、　　　　　　　１．ｏａｒＬｉＯＦＩ　　　　　　　２０　ｔＣｒｌｏｓ　　　　　　　α２ｆ２　実施例に同じＳ　ベリル添加と回転ベリルｔ−溶融塩中に浸漬さぜベルレ及びルツボをＩＲ
ＰＭＫて回転させ１０Ｈｒａ　　保持する。Example 2 1. Fiery purchasing solvent and blended beryl powder 10t v, o, 1. oar LiOFI 20 t Crlos α2f 2 Same as in Example S Beryl addition and rotation Beryl t-Immerse Beryl and crucible in molten salt IR
Rotate with PMK and hold for 10 hours.

４、　引上げ条件１０Ｈｒｓ　保持後α０５　ｍ　／’日の割合で１０日
間引上げを行った。その後、熱ショウＩＦＫて溶出処理
をし、合成エメナルドを得た。4. Pulling conditions: 10 hours After holding, pulling was carried out at a rate of α05 m/'day for 10 days. Thereafter, elution treatment was performed using hot IFK to obtain synthetic emerald.

Ｓ　結果及び所見Ｏ屈折率　　　１．５６８〜１．５６５０比　　重　　
　　　２．６５実施ＩＰＩＩ５１、　原料物質溶剤ならびに配合実施ガ１．に同じ２　＃融塩形成の澁度条件白金ルツボ内ンこ１材料を光」真して７５０’Ｃにて１
０　Ｈｒｍ保持する！Ｌ、　４ｉｊ実施例２に同じ５　結果及び所見Ｏ屈折率、比］ｌＦｉ実施例１に同じ実Ｊ１１１ＦＩＩ４ｔ　！Ｊ施ｆＰＵ１に同じ２、　１１１１１塩形成の１１１ＩＬ条件白會ルツボ内
に１の材料を充填して１２００℃にて５　Ｈｒｇの保持五　ベリル添加と回転ベリルを溶融塩中に浸漬させベリル及びルツボｆ２００
　ｒｐｍ　　ＶＣて回転させ２４　ＦＩｒｓ保持する４、　引上げ条件１０　Ｈｒｓ　　保持後α５−／日の割合で１０日間引
上げを行った。その後編水にて溶出処理をし合成エメラ
ルドｔ−得た。S Results and findings O Refractive index 1.568-1.5650 Specific gravity
2.65 Implementation IP II5 1. Raw material solvent and blending implementation 1. Same as 2 #Condition of molten salt formation: 1 material in platinum crucible was exposed to light at 750'C.
Maintain 0 Hrm! L, 4ij Same as Example 2 5 Results and Observations O Refractive Index, Ratio] lFi Same as Example 1 J111FII4 t! Same as PU1 2, 11111 Salt formation 111IL conditions Fill a white crucible with the material of 1 and hold at 1200℃ for 5 Hrg Addition of beryl and rotation Immerse beryl in molten salt Beryl and crucible f200
rpm VC and held for 24 FIrs 4. After holding for 10 Hrs, pulling was performed for 10 days at a rate of α5-/day. Thereafter, an elution treatment was performed using diluted water to obtain synthetic emerald T-.

＆　結果及び所見０屈折率、比重は実施例１に同じ。& Results and findings The zero refractive index and specific gravity are the same as in Example 1.

なお例示の実施例はベリルの回転数、引上げスピード、
濁度等の実施例以′外のものを或は既述の範囲のものを
選択して用いることも可能でめシ、本発明ｔｉ例示の実
施例に限定されることなく多くの変更代替付加が特許請
求の範囲會逸脱しない範囲で取捨選択できるものである
。In addition, the illustrated example is the rotation speed of beryl, the pulling speed,
It is also possible to select and use turbidity values other than those described in the examples or those within the range described above, and the present invention is not limited to the illustrative examples, but may be modified, substituted, or added. may be selected without departing from the scope of the claims.

以上の説明ならびに実施例よシ既に理博されたように本
発明によれに、従来の溶融塩法による人工ベリル単結晶
の合成法に簡単な引上げ装置を加えることによシ従来の
溶融地法の有する本質的利益上留保した上で品質の向上
ならびに収率の増大に着しく寄与してコストダウンを凶
れるので本発明は人工ベリル単結晶の合成法として極め
て有意義である。As already explained in the above description and examples, the present invention can be used to synthesize artificial beryl single crystals using the conventional molten salt method by adding a simple pulling device to the conventional molten salt method. The present invention is extremely significant as a method for synthesizing artificial beryl single crystals, since it significantly contributes to quality improvement and yield increase, and reduces costs, while retaining the essential benefits of the invention.

【図面の簡単な説明】[Brief explanation of the drawing]

第１図は不発ｋＪＡに基づく引上は床装置の断面図■　
添加ベリル固定及び引上げ１転シヤフト■　添加ベリル ■　ルツボ ■　耐火物 ■　ヒーター以　　　上第１［ｊ４Figure 1 is a cross-sectional view of the floor equipment for lifting based on unexploded kJA■
Added beryl fixing and pulling shaft ■ Added beryl ■ Crucible ■ Refractory ■ Heater and above 1st [j4

Claims

【特許請求の範囲】＋１１　　＃１ぼ天然ベリルの組成比を示す拳化ベリリ
ウム際化アルイニュウム、酸化シリコン及び酸化クロム
とその油の着色剤を加えてなる原料、または天然べＶル
粉末を原料にモリブデン酸、五酸化バナジウ＾、タンク
ステンｌＩ等よシ選ばれた１種又Ｆ１２種以上を加え加
熱溶融し溶融塩を形成させこの溶融塩中にベリル結晶を
添加、回転させ、引上げることＫよりベリルを合成し育
成することを特徴とする引上げ法による人工ベリルの合
成方法。（２）　　溶融塩より人工ベリルを合成し育成する方法
カヘリル結ａｔ添加し、Ｉ　ＲＰＭ〜２００ＲＰＭスピ
ードて回転することよりなる特許請求の範囲第１項虻載
の引上げ法ｅこよる人工ベリル単結晶の合成方法。（３）溶融塩よシ人工ベリル會合成し育成する方法がベ
リル結晶を添加しα０５〜α５　ｗｓ　／　ｄａｇのス
ピードで引上けることよりなる特許請求の範囲第１項記
載の引上げ法による人工ベリル単結晶の合成方法。（４）　　溶融塩よυ人工ベリルを合成し育成する方決
が溶融塩湯度分布よシなる特許１１１１ｊ求の範囲第１
ＪＪ記載の人工ベリル単結晶の合成方法。[Scope of Claims] +11 #1 A raw material obtained by adding a beryllium-based aluminum oxide having a composition ratio of #1 natural beryl, silicon oxide, chromium oxide, and its oil colorant, or a raw material made from natural beryl powder. Add one kind selected from molybdic acid, vanadium pentoxide, tanksten I, etc. or F12 or more, heat and melt to form a molten salt, add beryl crystals to the molten salt, rotate and pull. A method for synthesizing artificial beryl using a pulling method, which is characterized by synthesizing and growing beryl. (2) Method for synthesizing and growing artificial beryl from molten salt The pulling method described in claim 1, which comprises adding Caheryl crystals and rotating at a speed of I RPM to 200 RPM. synthesis method. (3) The method for synthesizing and growing artificial beryl using molten salt comprises adding beryl crystals and pulling it at a speed of α05 to α5 ws/dag. Method of synthesizing single crystals. (4) The method of synthesizing and growing artificial beryl from molten salt is based on the molten salt temperature distribution, which is the first scope of patent 1111j.
A method for synthesizing an artificial beryl single crystal as described in JJ.