JPH0159005B2 - - Google Patents

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Publication number
JPH0159005B2
JPH0159005B2 JP9470580A JP9470580A JPH0159005B2 JP H0159005 B2 JPH0159005 B2 JP H0159005B2 JP 9470580 A JP9470580 A JP 9470580A JP 9470580 A JP9470580 A JP 9470580A JP H0159005 B2 JPH0159005 B2 JP H0159005B2
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JP
Japan
Prior art keywords
deuterium
gas
metal
hydrogen
pressure
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
Application number
JP9470580A
Other languages
Japanese (ja)
Other versions
JPS5721921A (en
Inventor
Seijiro Suda
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.)
Individual
Original Assignee
Individual
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Filing date
Publication date
Application filed by Individual filed Critical Individual
Priority to JP9470580A priority Critical patent/JPS5721921A/en
Publication of JPS5721921A publication Critical patent/JPS5721921A/en
Publication of JPH0159005B2 publication Critical patent/JPH0159005B2/ja
Granted legal-status Critical Current

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Description

【発明の詳細な説明】 本発明は、重水素の濃縮分離方法、より詳しく
言えば、水素化物を形成しうる金属を用い、簡便
な操作で水素ガス中より効率よく重水素を濃縮分
離する新規な方法に関するものである。
DETAILED DESCRIPTION OF THE INVENTION The present invention provides a method for concentrating and separating deuterium, more specifically, a novel method for concentrating and separating deuterium more efficiently than in hydrogen gas using a metal that can form hydrides with simple operations. It concerns a method.

原子炉の減速体や冷却材として利用される重水
を形成し、核融合エネルギーの供給源として期待
されている重水素は、天然水を電気分解して得ら
れる重水素含有水素ガスから、遠心分離法あるい
は温度拡散法により分離することによつて得られ
てきた。しかしながら、この遠心分離法や温度拡
散法には、比較的高精度の装置を要し、装置が大
型化せざるを得ないという難点があつた。
Deuterium, which forms heavy water that is used as a moderator and coolant in nuclear reactors and is expected to be a source of fusion energy, is produced by centrifugation from deuterium-containing hydrogen gas obtained by electrolyzing natural water. It has been obtained by separation using the method or temperature diffusion method. However, the centrifugal separation method and the temperature diffusion method require relatively high-precision equipment, which has the disadvantage that the equipment has to be large in size.

本発明者らは、これらの難点を克服し、簡便な
操作で水素ガス中の重水素を効率よく濃縮分離で
きる方法を開発するために鋭意研究を重ねた結
果、水素化物を形成しうる金属を用いることによ
りその目的を達成しうることを見出し、本発明を
完成するに至つた。
The present inventors have conducted intensive research to overcome these difficulties and develop a method that can efficiently concentrate and separate deuterium in hydrogen gas using simple operations. The inventors have discovered that the object can be achieved by using the present invention, and have completed the present invention.

すなわち、本発明は、金属水素化物を形成しう
る金属に重水素含有ガスを供給し、金属水素化物
及び金属重水素化物を形成させたのち、金属重水
素化物の解離圧以上、金属水素化物の解離圧以下
の圧力下で金属水素化物を分解させ、放出された
水素を除去し、次いで、金属重水素化物を分解さ
せることを特徴とする重水素の濃縮分離方法を提
供するものである。
That is, in the present invention, a deuterium-containing gas is supplied to a metal capable of forming a metal hydride to form a metal hydride and a metal deuteride. The present invention provides a method for concentrating and separating deuterium, which is characterized by decomposing a metal hydride under a pressure equal to or lower than a dissociation pressure, removing released hydrogen, and then decomposing a metal deuteride.

本発明において用いられる金属としては金属水
素化物を形成しうるものであれば特に制限はな
く、例えば、ランタン・ニツケル系合金、ミツシ
ユメタル・ニツケル系合金、ミツシユメタル・ニ
ツケル・アルミニウム系合金、バナジウム、バナ
ジウム・ニオブ系合金、鉄・チタン系合金、チタ
ン・マンガン系合金、マグネシウム、マグネシウ
ム・銅系合金、マグネシウム・ニツケル系合金、
ランタン・コバルト系合金などを挙げることがで
きる。金属水素化物を形成しうるこれらの金属
は、重水素とも化合して金属重水素化合物を形成
する。本発明方法においては、金属水素化物を形
成しうる金属の一種又は二種以上が用いられ、用
いるに際しては、金属を活性化処理することが好
ましい。この活性化処理は、減圧下におかれた該
金属に水素ガスを供給して金属水素化物を形成さ
せ、次いで、減圧下において水素を放出させる操
作を、通常、数回から数十回繰り返すことにより
行われる。
The metal used in the present invention is not particularly limited as long as it can form a metal hydride; for example, lanthanum-nickel alloy, Mitsushimetal-nickel alloy, Mitsushimetal-nickel-aluminum alloy, vanadium, vanadium-nickel alloy, etc. Niobium alloys, iron/titanium alloys, titanium/manganese alloys, magnesium, magnesium/copper alloys, magnesium/nickel alloys,
Examples include lanthanum-cobalt alloys. These metals that can form metal hydrides also combine with deuterium to form metal deuterium compounds. In the method of the present invention, one or more metals capable of forming metal hydrides are used, and when used, it is preferable to activate the metals. In this activation process, hydrogen gas is supplied to the metal under reduced pressure to form a metal hydride, and then hydrogen is released under reduced pressure, which is usually repeated several to several dozen times. This is done by

本発明方法は、金属水素化物を形成しうる金属
に重水素含有ガスを供給し、金属を水素及び重水
素と化合させて金属水素化物及び金属重水素化物
とすることにより開始される。
The process of the present invention begins by supplying a deuterium-containing gas to a metal capable of forming metal hydrides and combining the metal with hydrogen and deuterium to form metal hydrides and metal deuterides.

このようにして得られた、金属水素化物及び金
属重水素化物を、次に、金属重水素化物の解離圧
以上、金属水素化物の解離圧以下の条件下にお
き、金属水素化物のみを分解させて、水素を放出
させ、放出された水素を系外に除去する。
The metal hydride and metal deuteride thus obtained are then placed under conditions that are higher than the dissociation pressure of the metal deuteride and lower than the dissociation pressure of the metal hydride, so that only the metal hydride is decomposed. to release hydrogen, and remove the released hydrogen from the system.

次いで、ガス雰囲気を金属重水素化物の解離圧
以下の圧力条件とし、金属重水素化物を分解させ
て重水素を放出させる。
Next, the gas atmosphere is set to a pressure condition below the dissociation pressure of the metal deuteride to decompose the metal deuteride and release deuterium.

このようにして重水素含有ガスは濃縮され、重
水素濃度が高められ、同様の操作を2〜3回繰り
返すことにより、数%程の重水素含有ガスを90%
以上の重水素含有ガスに濃縮することができる。
したがつて、本発明方法によれば、極めて微量の
重水素含有ガスからでも、簡便な操作で効率よく
重水素含有量の多いガスを得ることができる。
In this way, the deuterium-containing gas is concentrated and the deuterium concentration is increased, and by repeating the same operation two or three times, the deuterium-containing gas from several percent to 90%.
It can be concentrated to a deuterium-containing gas.
Therefore, according to the method of the present invention, a gas with a high deuterium content can be efficiently obtained with a simple operation even from an extremely small amount of deuterium-containing gas.

本発明方法の具体的実施は、例えば、反応圧力
容器、圧縮器、重水素含有ガス供給管、水素ガス
排気管、重水素ガス分離管及び不純物ガス排気管
などからなる濃縮装置を用いて行うことができ
る。すなわち、活性化された金属を反応圧力容器
に入れ、これに圧縮器を介して重水素含有高圧ガ
スを供給する。その供給圧力は、用いる金属の種
類や操作温度によつて異なり、また、不純物ガス
の有無によつても異なる。例えば、通常、不純物
ガスを含有する場合には、10〜50気圧程度の比較
的高圧が選ばれるが、不純物ガスを含まず、水素
と重水素との混合ガスである場合には、2〜5気
圧程度の圧力が選ばれる。
The method of the present invention can be specifically carried out using a concentrating device comprising, for example, a reaction pressure vessel, a compressor, a deuterium-containing gas supply pipe, a hydrogen gas exhaust pipe, a deuterium gas separation pipe, and an impurity gas exhaust pipe. Can be done. That is, the activated metal is placed in a reaction pressure vessel, and a high pressure gas containing deuterium is supplied to this via a compressor. The supply pressure varies depending on the type of metal used and the operating temperature, and also varies depending on the presence or absence of impurity gas. For example, if the gas contains an impurity gas, a relatively high pressure of about 10 to 50 atm is usually selected, but if the gas is a mixture of hydrogen and deuterium and does not contain an impurity gas, a relatively high pressure of about 2 to 50 atm is selected. A pressure of about atmospheric pressure is selected.

このガス供給により、金属が金属水素化物及び
金属重水素化物となつたのち、反応圧力容器中に
残存する不純物ガスを不純物ガス排気管により排
除する。この際、排気は、金属水素化物を解離さ
せないため、瞬間的に行うことが好ましい。供給
ガスがこのような不純物ガスを含有しない場合に
は、この工程は不要である。
After the metal is converted into a metal hydride and a metal deuteride by this gas supply, the impurity gas remaining in the reaction pressure vessel is removed by the impurity gas exhaust pipe. At this time, evacuation is preferably performed instantaneously so as not to dissociate the metal hydride. If the feed gas does not contain such impurity gases, this step is not necessary.

次いで、所定圧力下で金属水素化物を分解さ
せ、放出された反応圧力容器中の水素を水素ガス
排気管より排除し、その後、反応圧力容器中の圧
力を金属重水素化物の解離圧以下に低下させて金
属重水素化物を分解させ、放出された重水素を重
水素分離管を介して採取する。
Next, the metal hydride is decomposed under a predetermined pressure, the released hydrogen in the reaction pressure vessel is removed from the hydrogen gas exhaust pipe, and then the pressure in the reaction pressure vessel is lowered to below the dissociation pressure of the metal deuteride. The metal deuteride is decomposed, and the released deuterium is collected through a deuterium separation tube.

このようにして、1回の操作で得られる重水素
の濃縮ガスを再び反応圧力容器に供給し、同様の
操作を繰り返すことによりさらに濃縮することが
できる。
In this way, the deuterium concentrated gas obtained in one operation can be supplied again to the reaction pressure vessel and further concentrated by repeating the same operation.

他方、供給ガスが不純物ガスを含まず、水素ガ
スと重水素ガスからなり、その重水素ガス濃度が
低い場合には、初段階的濃縮を、混合ガス中の水
素ガスのみを金属に吸蔵させることによつても行
うことができる。すなわち、この場合は、金属に
吸蔵される水素の速度が重水素に比べて速いの
で、混合ガス中の水素ガスを優先的に吸蔵させ、
残存ガス中の重水素濃度を高める方法である。こ
の方法は、濃縮処理時間の短縮を図りうる点で有
利である。
On the other hand, if the supplied gas does not contain impurity gases but is composed of hydrogen gas and deuterium gas, and the deuterium gas concentration is low, initial concentration is performed by occluding only the hydrogen gas in the mixed gas into the metal. This can also be done by In other words, in this case, the rate of hydrogen occlusion in the metal is faster than that of deuterium, so hydrogen gas in the mixed gas is preferentially occluded,
This is a method of increasing the deuterium concentration in residual gas. This method is advantageous in that the concentration treatment time can be shortened.

また、本発明方法により濃縮された重水素ガス
を金属重水素化物として貯蔵、運搬することがで
き、簡便な重水素供給源とすることができる。
Further, the deuterium gas concentrated by the method of the present invention can be stored and transported as a metal deuteride, and can be used as a simple deuterium supply source.

次に、実施例により本発明をさらに詳細に説明
する。
Next, the present invention will be explained in more detail with reference to Examples.

実施例 1 第1図にその概念図として示した装置及び室温
で約10-2Torrの真空下におき、次いで20気圧の
水素圧下において水素を吸蔵させる操作を3回繰
り返して活性化させたランタン・ニツケル合金
(LaNi5)を用い、このLaNi5500gを反応器2に
充てんし、これに重水素5モル%、水素75モル
%、その他20モル%からなる混合ガスを圧縮器1
により30気圧に圧縮して供給し、15℃の温度にお
いて反応させた。反応終了後、不純物ガス排気管
バルブ3を瞬間的に開閉して反応器内圧力を約1
気圧に下げ、不純物ガスを排気した。このとき、
反応器内の混合ガス組成(LaNi5−H、LaNi5
Dとなつているものを含む)は、D2:H2:不純
物ガス=6.24:93.64:0.12(モル%)であつた。
Example 1 The apparatus shown as a conceptual diagram in Fig. 1 and a lantern activated by placing it under a vacuum of about 10 -2 Torr at room temperature and then storing hydrogen under a hydrogen pressure of 20 atmospheres were repeated three times.・Using a nickel alloy (LaNi 5 ), 500 g of this LaNi 5 is filled in reactor 2, and a mixed gas consisting of 5 mol% deuterium, 75 mol% hydrogen, and 20 mol% of others is added to compressor 1.
The reactor was compressed to 30 atmospheres and reacted at a temperature of 15°C. After the reaction is completed, the impurity gas exhaust pipe valve 3 is opened and closed momentarily to reduce the pressure inside the reactor to approximately 1.
The pressure was lowered and impurity gases were evacuated. At this time,
Mixed gas composition in the reactor (LaNi 5 −H, LaNi 5
(including those marked with D) was D2 : H2 :impurity gas=6.24:93.64:0.12 (mol%).

次いで、水素ガス排気バルブ4を開き、反応器
内圧力を約1.05気圧(800mmHg)に保持しながら
除々に水素を排気し、LaNi5−Hの解離圧が反応
器内圧力と等しくなつたとき、水素ガス排気バル
ブを閉じた。そして、重水素分離バルブ5を開
き、重水素の濃縮水素混合ガスを得た。この混合
ガス組成はD2:H2=33.4:66.6(モル%)であり、
不純物ガス含有量は10ppm以下であつた。
Next, the hydrogen gas exhaust valve 4 was opened to gradually exhaust hydrogen while maintaining the pressure inside the reactor at about 1.05 atmospheres (800 mmHg), and when the dissociation pressure of LaNi 5 -H became equal to the pressure inside the reactor, The hydrogen gas exhaust valve was closed. Then, the deuterium separation valve 5 was opened to obtain a concentrated hydrogen mixed gas of deuterium. This mixed gas composition is D2 : H2 =33.4:66.6 (mol%),
The impurity gas content was 10 ppm or less.

次に、このようにして得られた、重水素を33.4
モル%含有する水素ガスを、圧縮器で3気圧に圧
縮して反応器に再び供給し、LaNi5と反応させた
のち、水素ガス排気バルブを開き、反応器内圧力
を約1.05気圧に保持しながら除々に水素を排気さ
せ、所定圧力におけるLaNi5−Hの分解が終了し
たとき水素ガス排気バルブを閉じ、重水素分離バ
ルブを開いた。この二度目の操作により得られた
ガス中の重水素濃度は78.8モル%であつた。この
ガスを供給ガスとして、さらにもう一度同様の操
作を繰り返すことにより得られたガス中の重水素
濃度は96.1モル%であつた。
Next, the deuterium obtained in this way is 33.4
Hydrogen gas containing mol% was compressed to 3 atm using a compressor and supplied to the reactor again to react with LaNi 5. After that, the hydrogen gas exhaust valve was opened and the pressure inside the reactor was maintained at approximately 1.05 atm. While doing so, hydrogen was gradually exhausted, and when the decomposition of LaNi 5 --H at a predetermined pressure was completed, the hydrogen gas exhaust valve was closed and the deuterium separation valve was opened. The deuterium concentration in the gas obtained by this second operation was 78.8 mol%. The same operation was repeated once again using this gas as the feed gas, and the deuterium concentration in the gas obtained was 96.1 mol%.

なお、LaNi5−H及びLaNi5−Dの0℃、10℃
及び15℃における解離圧特性を第2図に示す。
In addition, LaNi 5 -H and LaNi 5 -D at 0°C and 10°C
Figure 2 shows the dissociation pressure characteristics at 15°C and 15°C.

実施例 2 実施例1で用いた装置及びLaNi5の場合と同様
にして活性化したバナジウム(V)を用い、反応
器に充てんしたV500gに、D210モル%、H250モ
ル%、不純物ガス40モル%からなる混合ガスを30
気圧に圧縮して供給し、Vと反応させ、不純物ガ
スを瞬間的に排気した。このときの混合ガス組成
(V−H及びV−Dとしてのものを含む)は、
D2:H2不純物ガス=15.15:84.83:0.02(モル%)
であつた。
Example 2 Using the equipment used in Example 1 and vanadium (V) activated in the same manner as in the case of LaNi 5 , 500 g of V filled in a reactor was charged with 10 mol% of D 2 , 50 mol% of H 2 , and impurities. A mixture of gases consisting of 40 mol% of 30
It was compressed to atmospheric pressure and supplied, reacted with V, and impurity gas was instantly exhausted. The mixed gas composition at this time (including those as V-H and V-D) is
D2 : H2 impurity gas = 15.15:84.83:0.02 (mol%)
It was hot.

次いで、反応器内水素圧を3気圧に保持して、
V−Hを分解し、放出された水素を排気した。分
解終了後、反応器内水素圧を1気圧に下げてV−
Dを分解させ、重水素濃度が50.5モル%の濃縮ガ
スを得た。この得られた濃縮ガスを5気圧に圧縮
して再び反応器内に供給し、反応終了後、反応器
内圧力を3気圧に下げてV−Hを分解し、分解終
了後、反応器内圧力を1気圧に下げてV−Dを分
解した。得られたガス中の重水素濃度は92.9モル
%であつた。
Next, the hydrogen pressure inside the reactor was maintained at 3 atm,
The V-H was decomposed and the released hydrogen was vented. After the decomposition is completed, the hydrogen pressure inside the reactor is lowered to 1 atm and V-
D was decomposed to obtain a concentrated gas with a deuterium concentration of 50.5 mol%. The obtained concentrated gas is compressed to 5 atm and fed into the reactor again, and after the reaction is finished, the pressure inside the reactor is lowered to 3 atm to decompose V-H. V-D was decomposed by lowering the pressure to 1 atm. The deuterium concentration in the obtained gas was 92.9 mol%.

なお、操作は全て40℃の温度において行つた。
また、第3図にV−H及びV−Dの40℃における
解離圧特性を示す。
Note that all operations were performed at a temperature of 40°C.
Further, FIG. 3 shows the dissociation pressure characteristics of VH and VD at 40°C.

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

第1図は、本発明方法の実施に用いられる装置
の一例を示す概念図であり、図中、1は圧縮器、
2は反応器、3は不純物ガス排気バルブ、4は水
素ガス排気バルブ、5は重水素分離バルブをそれ
ぞれ示す。 また、第2図は、0℃(a)、10℃(b)及び15℃(c)に
おけるランタン・ニツケル合金、第3図は40℃に
おけるバナジウムの水素(実線)及び重水素(破
線)の解離圧特性を表わすグラフであり、図中、
縦軸は圧力(気圧)、横軸は金属1モル当りの水
素又は重水素の吸蔵モル数を表わす。
FIG. 1 is a conceptual diagram showing an example of an apparatus used to carry out the method of the present invention, in which 1 is a compressor;
2 is a reactor, 3 is an impurity gas exhaust valve, 4 is a hydrogen gas exhaust valve, and 5 is a deuterium separation valve. Figure 2 shows the hydrogen (solid line) and deuterium (dashed line) of vanadium at 40°C. It is a graph showing dissociation pressure characteristics, and in the figure,
The vertical axis represents pressure (atmospheric pressure), and the horizontal axis represents the number of moles of hydrogen or deuterium absorbed per mole of metal.

Claims (1)

【特許請求の範囲】[Claims] 1 金属水素化物および金属重水素化物を形成し
うる金属に重水素含有ガスを供給し、金属水素化
物及び金属重水素化物を形成させたのち、金属重
水素化物の解離圧以上、金属水素化物の解離圧以
下の圧力下で金属水素化物を分解させ、放出され
た水素を除去し、次いで、金属重水素化物を分解
させることを特徴とする重水素の濃縮分離方法。
1. After supplying a deuterium-containing gas to a metal capable of forming metal hydrides and metal deuterides to form metal hydrides and metal deuterides, A method for concentrating and separating deuterium, which comprises decomposing a metal hydride under a pressure equal to or lower than a dissociation pressure, removing released hydrogen, and then decomposing a metal deuteride.
JP9470580A 1980-07-11 1980-07-11 Concentration and separation method of heavy hydrogen Granted JPS5721921A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP9470580A JPS5721921A (en) 1980-07-11 1980-07-11 Concentration and separation method of heavy hydrogen

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP9470580A JPS5721921A (en) 1980-07-11 1980-07-11 Concentration and separation method of heavy hydrogen

Publications (2)

Publication Number Publication Date
JPS5721921A JPS5721921A (en) 1982-02-04
JPH0159005B2 true JPH0159005B2 (en) 1989-12-14

Family

ID=14117572

Family Applications (1)

Application Number Title Priority Date Filing Date
JP9470580A Granted JPS5721921A (en) 1980-07-11 1980-07-11 Concentration and separation method of heavy hydrogen

Country Status (1)

Country Link
JP (1) JPS5721921A (en)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS63205127A (en) * 1987-02-20 1988-08-24 Sumitomo Heavy Ind Ltd Device for hydrogen isotope separate concentration

Also Published As

Publication number Publication date
JPS5721921A (en) 1982-02-04

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