JP2008266662A - Molten salt electrolytic refiner and molten salt electrolytic refining method - Google Patents

Molten salt electrolytic refiner and molten salt electrolytic refining method Download PDF

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JP2008266662A
JP2008266662A JP2007106891A JP2007106891A JP2008266662A JP 2008266662 A JP2008266662 A JP 2008266662A JP 2007106891 A JP2007106891 A JP 2007106891A JP 2007106891 A JP2007106891 A JP 2007106891A JP 2008266662 A JP2008266662 A JP 2008266662A
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liquid metal
molten salt
metal cathode
crucible
cathode
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JP5016964B2 (en
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Hitoshi Nakamura
等 中村
Reiko Fujita
玲子 藤田
Yukimoto Fuse
行基 布施
Akihiro Kawabe
晃寛 川辺
Kazuhiro Utsunomiya
一博 宇都宮
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract

<P>PROBLEM TO BE SOLVED: To efficiently recover a large amount of U and TRU without increasing an amount of liquid metal used as an anode by steadily maintaining the interface of a liquid metal electrode of a molten salt electrolytic refiner to an original composition. <P>SOLUTION: The molten salt electrolytic refiner having an electrolytic cell installed in an electric furnace and housed with a molten salt, an anode container charged with a used nuclear fuel, and a liquid metal crucible housed with liquid metal cathode is equipped with a compressive apparatus which compresses the solid precipitated object generated at the interface of the liquid metal cathode to a liquid metal cathode bottom. <P>COPYRIGHT: (C)2009,JPO&INPIT

Description

本発明は使用済み核燃料の乾式再処理技術に関し、特に、使用済み核燃料中に含まれるウラン（Ｕ）及び超ウラン元素（ＴＲＵ）を電解精製により同時に回収し再利用するための溶融塩電解精製装置及び溶融塩電解精製方法に関する。   The present invention relates to a dry reprocessing technique for spent nuclear fuel, and in particular, a molten salt electrorefining apparatus for simultaneously recovering and reusing uranium (U) and transuranium element (TRU) contained in spent nuclear fuel by electrolytic purification. And a molten salt electrolytic purification method.

従来、使用済み核燃料は硝酸に溶解して有機溶媒により、核分裂生成物を除去し、価数を調整することにより、酸化ウランや酸化プルトニウムを分けて回収するピューレックス法が開発されていた。しかしながらピューレックス法に代表される湿式再処理技術は、大規模な設備を必要とし、また、廃棄物が大量に発生するので、最近では設備の小型化が可能で廃棄物の発生量も少ない乾式再処理技術が開発されてきている。   Conventionally, a purex process has been developed in which spent nuclear fuel is dissolved in nitric acid, the fission products are removed with an organic solvent, and the valence is adjusted to separate and recover uranium oxide and plutonium oxide. However, the wet reprocessing technology represented by the PUREX method requires large-scale equipment and generates a large amount of waste. Therefore, recently, it is possible to reduce the size of the equipment and to reduce the amount of waste generated. Reprocessing techniques have been developed.

乾式再処理技術の中で、溶融塩電解精製法により使用済み核燃料を処理する方法は、溶融塩中に設置され、陽極として機能する使用済み核燃料が収納される容器と、固体陰極と、Ｃｄ等の溶融金属からなる液体金属陰極と、から構成される電解精製装置を用い、使用済み核燃料を電解で陽極溶解した後、金属ウランを固体陰極に回収し、さらに、溶融塩中に残存するウラン（Ｕ）、プルトニウム（Ｐｕ）およびマイナーアクチニド（ＭＡ：ネプツニウム（ＮＰ）、アメリシウム（Ａｍ）、キュリウム（Ｃｍ））を液体金属陰極で回収する（特許文献１の図４参照）。   Among dry reprocessing technologies, a method of treating spent nuclear fuel by molten salt electrorefining is a method of installing a spent nuclear fuel installed in molten salt and functioning as an anode, a solid cathode, Cd, etc. And using a liquid metal cathode composed of a molten metal, and anodic dissolution of spent nuclear fuel by electrolysis, and then recovering the metal uranium to a solid cathode, and further uranium remaining in the molten salt ( U), plutonium (Pu), and minor actinides (MA: neptunium (NP), americium (Am), curium (Cm)) are recovered with a liquid metal cathode (see FIG. 4 of Patent Document 1).

しかしながら、このような溶融塩電解法による電解精製装置では、電解が進行すると液体金属陰極中のＵ及びＴＲＵ濃度が上昇し、その濃度が飽和濃度を超えると液体金属陰極の界面にＵ及びＴＲＵの固体析出物が析出し始める。この状態になると液体金属陰極は固体陰極として作用することになって、Ｕのみが選択的に析出することになり、その結果、回収効率が低下するとともにＵ及びＴＲＵの同時回収が出来なくなる。   However, in such an electrorefining apparatus using the molten salt electrolysis method, the U and TRU concentrations in the liquid metal cathode increase as electrolysis proceeds, and when the concentration exceeds the saturation concentration, the U and TRU concentration is increased at the interface of the liquid metal cathode. Solid precipitate begins to precipitate. In this state, the liquid metal cathode acts as a solid cathode, so that only U is selectively deposited. As a result, the recovery efficiency is lowered and U and TRU cannot be recovered simultaneously.

この問題に対処し、液体金属陰極表面にウラン、プルトニウムが過度に析出蓄積するのを防ぐため、従来からいろいろな対策が検討されてきた。例えば、液体金属陰極に液体金属を攪拌するための攪拌手段を設ける（特許文献１〜３）、又は析出したウラン、プルトニウムを微粒子化（パウンダリング）するための微粒子化手段（特許文献４）を設ける等の対策が講じられている。
特開平７−１６７９８５号公報 特開平９−２５７９８６号公報 特開平１０−２９３１９３号公報 特開平１１−１４８９９６号公報 In order to cope with this problem and prevent uranium and plutonium from excessively depositing and accumulating on the surface of the liquid metal cathode, various countermeasures have been studied. For example, a liquid metal cathode is provided with a stirring means for stirring the liquid metal (Patent Documents 1 to 3), or a microparticulating means (Patent Document 4) for micronizing (pouring) the precipitated uranium and plutonium. Measures such as establishment are taken.
JP-A-7-167985 JP-A-9-257986 Japanese Patent Laid-Open No. 10-293193 JP-A-11-148996

上記従来の方法は、液体金属陰極の界面を操作するものであり、電解精製中、頻繁に撹拌装置等を操作しなければならないとともに、液体金属陰極の界面に析出する固体析出物をその界面から実質的に除去するものではなく、精製が進行するにつれて回収効率が低下し、その結果、Ｕ及びＴＲＵを同時にかつ大量に回収することが困難となっていた。   The above-described conventional method is to operate the interface of the liquid metal cathode. During the electrolytic purification, the stirrer and the like must be operated frequently, and solid precipitates deposited on the interface of the liquid metal cathode are removed from the interface. It was not substantially removed, and the recovery efficiency decreased as purification progressed. As a result, it was difficult to recover U and TRU in large quantities simultaneously.

さらに、溶融塩電解精製装置の商業的稼働を可能とするためには、液体金属陰極界面へのＵ、ＰｕおよびＭＡ金属の析出蓄積を防止しつつ液体金属陰極へのＵ、ＰｕおよびＭＡの液体金属への回収量を高くする必要があるが、上記従来の方法では対応できなかった。   Furthermore, in order to enable commercial operation of the molten salt electrorefining apparatus, U, Pu and MA liquids on the liquid metal cathode while preventing deposition of U, Pu and MA metals on the liquid metal cathode interface. Although it is necessary to increase the recovery amount to the metal, the conventional method cannot cope with it.

また、従来の溶融塩電解精製方法は、電解精製が進行具合に応じて液体金属陰極を液体金属陰極ルツボごと取り出し、後処理によりＵ及びＴＲＵを回収する方法であり、液体金属陰極ルツを取り出す度に電解槽の運転を停止する必要があり、Ｕ及びＴＲＵの回収効率が低下させ、回収コストも高いものとなっていた。   Further, the conventional molten salt electrolytic purification method is a method in which the liquid metal cathode is taken out together with the liquid metal cathode crucible according to the progress of the electrolytic purification, and U and TRU are recovered by post-processing. In addition, it is necessary to stop the operation of the electrolytic cell, the recovery efficiency of U and TRU is lowered, and the recovery cost is high.

本発明の目的は、Ｕ及びＴＲＵを使用済み核燃料から分離し、低融点の液体金属陰極を用いてＵ、ＴＲＵを同時に回収する溶融塩電解精製装置及びその方法において、液体金属陰極の界面に析出蓄積する固体析出物を圧縮分離する新規な圧縮装置構造を採用したことにより、常に液体金属電極の界面を本来の液体金属陰極組成に定常的に維持し、陰極として使用する液体金属量を増大させることなく大量のＵ、ＴＲＵを回収できる溶融塩電解精製装置及びその方法を提供する。   It is an object of the present invention to separate U and TRU from spent nuclear fuel and to deposit U and TRU at the same time using a low-melting-point liquid metal cathode. By adopting a new compression device structure that compresses and separates accumulated solid precipitates, the interface of the liquid metal electrode is constantly maintained at the original liquid metal cathode composition, and the amount of liquid metal used as the cathode is increased. Disclosed are a molten salt electrorefining apparatus and a method for recovering a large amount of U and TRU without any problems.

上記目的を達成するために、本発明は溶融塩が収容された電解槽と、使用済み核核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する溶融塩電解精製装置において、前記液体金属陰極の界面に発生する固体析出物を液体金属陰極底部に圧縮する昇降可能な圧縮装置を備えたことを特徴とする。   In order to achieve the above object, the present invention provides an electrolytic cell containing a molten salt, an anode container loaded with spent nuclear nuclear fuel, and a liquid metal crucible containing a liquid metal cathode. The refining apparatus is characterized by comprising a compressing device capable of moving up and down to compress the solid precipitate generated at the interface of the liquid metal cathode to the bottom of the liquid metal cathode.

また、本発明は溶融塩が収容された電解槽と、使用済み核核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する溶融塩電解精製装置において、前記液体金属陰極の界面に発生する固体析出物を液体金属陰極底部に圧縮する昇降可能な圧縮装置と、前記液体金属ルツボの内側に設けられた内側容器と、を備えたことを特徴とする。   The present invention also relates to a molten salt electrorefining apparatus comprising: an electrolytic cell containing a molten salt; an anode container loaded with a spent nuclear nuclear fuel; and a liquid metal crucible containing a liquid metal cathode. A compression device capable of moving up and down for compressing solid precipitates generated at the interface of the metal cathode to the bottom of the liquid metal cathode, and an inner container provided inside the liquid metal crucible are provided.

また、本発明は溶融塩が収容された電解槽と、使用済み核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する使用済み核燃料の溶融塩電解精製方法において、下部にメッシュまたは焼結金属等からなるフィルターが設けられた圧縮装置を液体金属陰極内に下降させ、前記液体金属陰極の界面に発生する固体析出物を前記液体金属陰極底部に圧縮することを特徴とする。   The present invention also relates to a molten salt electrorefining method for spent nuclear fuel comprising an electrolytic cell containing molten salt, an anode container loaded with spent nuclear fuel, and a liquid metal crucible containing a liquid metal cathode. Lowering the compression device provided with a filter made of mesh or sintered metal or the like in the lower part into the liquid metal cathode and compressing the solid precipitate generated at the interface of the liquid metal cathode to the bottom of the liquid metal cathode. Features.

さらに、本発明は溶融塩が収容された電解槽と、使用済み核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する使用済み核燃料の溶融塩電解精製方法において、下部にメッシュまたは焼結金属等からなるフィルターが設けられた圧縮装置を前記液体金属陰極内に下降させ、前記圧縮装置と前記液体金属ルツボの内側に設けられた内側容器とを係合し、前記圧縮装置と前記内側容器を係合させた状態で前記圧縮装置を引き上げることを特徴とする。   Furthermore, the present invention relates to a method for electrolytically refining a spent nuclear fuel with a molten salt, an anode container loaded with a spent nuclear fuel, and a liquid metal crucible containing a liquid metal cathode. A compression device provided with a filter made of mesh or sintered metal at the lower part is lowered into the liquid metal cathode, and the compression device and an inner container provided inside the liquid metal crucible are engaged, The compression device is pulled up with the compression device and the inner container engaged.

本発明による使用済み核燃料の溶融塩電解精製装置及びその方法によれば、常に液体金属電極の界面を本来の液体金属陰極組成に定常的に維持し、陰極として使用する液体金属量を増大させることなく大量のＵ及びＴＲＵを効率的に回収できる。また、液体金属陰極に使用する液体金属の単位体積あたりのＵ及びＴＲＵの回収量を格段に向上させることができるので回収コストを大幅に低くすることができ、その結果、本発明に係る装置を商業的に稼働させることが可能となる。   According to the molten salt electrorefining apparatus and method for spent nuclear fuel according to the present invention, the interface of the liquid metal electrode is constantly maintained at the original liquid metal cathode composition, and the amount of liquid metal used as the cathode is increased. A large amount of U and TRU can be efficiently recovered. Moreover, since the recovery amount of U and TRU per unit volume of the liquid metal used for the liquid metal cathode can be remarkably improved, the recovery cost can be greatly reduced. As a result, the apparatus according to the present invention can be reduced. It can be operated commercially.

以下、本発明に係る溶融塩電解精製装置及びその方法の実施の形態について図を参照して説明する。   Embodiments of a molten salt electrolytic purification apparatus and method according to the present invention will be described below with reference to the drawings.

（第１の実施の形態）
本発明に係る第１の実施の形態を図１および図２を用いて説明する。
図１は、本発明に係る溶融塩電解精製装置の構成を示したものである。
図１において、加熱溶融状態の溶融塩３は電気炉１内に設置された電解槽２中に収容されている。この溶融塩３中に使用済み核燃料４が装荷された陽極容器５と絶縁材料で形成され液体金属陰極６を収容する液体金属ルツボ７が設置されている。 (First embodiment)
A first embodiment according to the present invention will be described with reference to FIGS.
FIG. 1 shows the configuration of a molten salt electrolytic purification apparatus according to the present invention.
In FIG. 1, a molten salt 3 in a heated and melted state is accommodated in an electrolytic cell 2 installed in an electric furnace 1. An anode container 5 loaded with spent nuclear fuel 4 in the molten salt 3 and a liquid metal crucible 7 formed of an insulating material and containing a liquid metal cathode 6 are installed.

液体金属陰極６の内部には下部がメッシュまたは焼結金属等からなるフィルター８ａを具備する内側容器８が設置されている。また、液体金属陰極ルツボ７は同様の絶縁材料で形成されたルツボ外容器９に収納される。当該液体金属陰極ルツボ７の直上には下部がメッシュまたは焼結金属等からなるフィルター１０ａを具備する圧縮装置１０が設置され、図示しない駆動装置により昇降可能となっている。陽極容器５と液体金属陰極６の間には電源１１が接続されこれにより過電圧を加えることで陽極−陰極間に電流が流れ、陽極ではＵ、ＴＲＵが溶解され液体金属陰極６ではＵ、ＴＲＵが精製還元される。   Inside the liquid metal cathode 6, an inner container 8 having a filter 8a whose lower part is made of mesh or sintered metal is installed. Further, the liquid metal cathode crucible 7 is housed in a crucible outer container 9 made of the same insulating material. Immediately above the liquid metal cathode crucible 7, a compression device 10 having a filter 10a whose lower portion is made of mesh or sintered metal is installed and can be moved up and down by a driving device (not shown). A power source 11 is connected between the anode vessel 5 and the liquid metal cathode 6, whereby an overvoltage is applied to cause a current to flow between the anode and the cathode. U and TRU are dissolved at the anode, and U and TRU are dissolved at the liquid metal cathode 6 Purified and reduced.

このように構成された装置において、陽極容器５中の使用済み核燃料４から溶融し溶融塩３中に拡散したＵ、ＴＲＵイオンは陰極で金属に還元され速やかに溶融金属陰極６に溶解するが、電解が進行し溶融金属陰極６中のＵ、ＴＲＵ濃度が上昇して飽和濃度を超えると溶融金属陰極６の界面にＵ、ＴＲＵの固体析出物１２が析出し始める。この状態が進むと液体金属陰極６は析出蓄積された固体析出物１２の存在により固体陰極として作用することになって、Ｕのみが選択的に析出することになり、その結果、Ｕ、ＴＲＵの同時回収ができなくなる。   In the apparatus configured as described above, U and TRU ions that are melted from the spent nuclear fuel 4 in the anode vessel 5 and diffused into the molten salt 3 are reduced to metal at the cathode and quickly dissolved in the molten metal cathode 6. When electrolysis progresses and the U and TRU concentrations in the molten metal cathode 6 increase and exceed the saturation concentration, the U and TRU solid precipitates 12 begin to deposit at the interface of the molten metal cathode 6. When this state proceeds, the liquid metal cathode 6 acts as a solid cathode due to the presence of the solid deposit 12 deposited and accumulated, so that only U is selectively deposited. As a result, U, TRU Simultaneous collection is impossible.

本発明の第１の実施の形態では、溶融金属陰極６の界面に析出した固体析出物１２を取り除くために、圧縮装置１０を図示しない駆動装置により降下させ液体金属陰極ルツボ７内内側容器小野８の中に挿入し、固体析出物１２を内側容器８の底部に圧縮する。このとき液体金属ルツボ７内の液体金属は圧縮装置１０の底部に設けられたメッシュまたは焼結金属等からなるフィルター１０ａを通って圧縮装置１０の内側に入り込む（図２（ａ））。そして、液体金属中の固形化した固体析出物１２のみが液体金属陰極ルツボ７内の内側容器８の底部に圧縮される（図２（ａ））。   In the first embodiment of the present invention, in order to remove the solid deposit 12 deposited on the interface of the molten metal cathode 6, the compression device 10 is lowered by a driving device (not shown) to inner container ono 8 in the liquid metal cathode crucible 7. The solid deposit 12 is compressed into the bottom of the inner container 8. At this time, the liquid metal in the liquid metal crucible 7 enters the inside of the compression device 10 through a filter 10a made of a mesh or a sintered metal provided at the bottom of the compression device 10 (FIG. 2A). Then, only the solid precipitate 12 solidified in the liquid metal is compressed to the bottom of the inner container 8 in the liquid metal cathode crucible 7 (FIG. 2A).

次に圧縮装置１０を引き上げたときには圧縮装置１０の底部に設けられたメッシュまたは焼結金属等からなるフィルター１０ａを通して、液体金属は再び陰極ルツボ７内に戻されることになる（図２（ｂ））。この操作により液体金属陰極６の界面は、金属Ｕ、ＴＲＵの固体析出物１２が存在しない状態を回復する。   Next, when the compression device 10 is pulled up, the liquid metal is returned again into the cathode crucible 7 through the filter 10a made of a mesh or sintered metal provided at the bottom of the compression device 10 (FIG. 2B). ). By this operation, the interface of the liquid metal cathode 6 recovers the state where the metal U and TRU solid precipitates 12 do not exist.

この第１の実施の形態によれば、圧縮装置１０の昇降動作により固体析出物１２を効率的に界面から除去できるので、常に液体電極陰極６の界面を固体析出物のない液体金属陰極組成に維持することが可能となり、これにより液体金属量を増大させることなく大量のＵ、ＴＲＵを同時に回収することができる。   According to the first embodiment, since the solid precipitate 12 can be efficiently removed from the interface by the lifting and lowering operation of the compression device 10, the interface of the liquid electrode cathode 6 is always made into a liquid metal cathode composition free of solid precipitate. Thus, a large amount of U and TRU can be recovered simultaneously without increasing the amount of liquid metal.

（第２の実施の形態）
本発明に係る第２の実施の形態を、図３を用いて説明する。
液体金属陰極ルツボ７内に配置された内側容器８に対し、上記圧縮装置１０による圧縮動作を繰り返し行うと、固体析出物１２は内側容器８の底部に徐々に堆積することになり、その結果、液体金属陰極界面はルツボ７内を次第に上昇する。この上昇した界面がルツボの縁を超えると回収したＵ、ＴＲＵは液体金属陰極ルツボ７の外側に落下しＵ、ＴＲＵの回収が困難になる。そこで液体金属陰極ルツボ７を収納するルツボ外容器９を液体金属陰極ルツボ７の周囲に設置することにより、液体金属陰極ルツボ７からあふれたＵ、ＴＲＵを含む液体金属をルツボ外容器９に回収する。 (Second Embodiment)
A second embodiment according to the present invention will be described with reference to FIG.
When the compression operation by the compression device 10 is repeatedly performed on the inner container 8 disposed in the liquid metal cathode crucible 7, the solid precipitate 12 is gradually deposited on the bottom of the inner container 8, and as a result, The liquid metal cathode interface gradually rises in the crucible 7. When the raised interface exceeds the edge of the crucible, the recovered U and TRU fall outside the liquid metal cathode crucible 7, making it difficult to recover U and TRU. Therefore, by installing a crucible outer container 9 for storing the liquid metal cathode crucible 7 around the liquid metal cathode crucible 7, the liquid metal containing U and TRU overflowing from the liquid metal cathode crucible 7 is collected in the crucible outer container 9. .

本第２の実施の形態によれば、液体金属陰極ルツボ７からあふれた液体金属を回収するルツボ外容器９を設けたことにより、さらに効率よく多くのＵ、ＴＲＵを回収することが可能となる。   According to the second embodiment, by providing the crucible outer container 9 for recovering the liquid metal overflowing from the liquid metal cathode crucible 7, it becomes possible to recover more U and TRU more efficiently. .

（第３の実施の形態）
第３の実施の形態を図４を用いて説明する。
内側容器８の底部に圧縮された固体析出物１２は、析出量が多くなると液体金属陰極の回収効率に悪影響を及ぼすので、適宜、電解槽２の外部に取り出す必要がある。そのために、圧縮装置１０と内側容器８とを図示しない着脱可能な係合手段により係合／取外し可能とする。なお、係合手段はフック等、通常の係合手段が用いられる。そして、固体析出物１２を電解槽２の外部に取り出すときは、圧縮装置１０と内側容器８を前記係合手段により係合し、固体析出物１２を内側容器８とともに液体金属陰極６内から引き上げ、固体析出物１２を回収する。これにより電解槽２の運転を停止することなく固体析出物１２を回収することができる。内側容器８の引き上げの際に、内側容器８内の液体金属は内側容器８下部に設けたメッシュまたは焼結金属等からなるフィルター８ａを通し陰極ルツボ内に戻され、再度陰極としての使用が可能となる。 (Third embodiment)
A third embodiment will be described with reference to FIG.
The solid precipitate 12 compressed on the bottom of the inner container 8 adversely affects the recovery efficiency of the liquid metal cathode when the amount of precipitation increases, and therefore needs to be taken out of the electrolytic cell 2 as appropriate. For this purpose, the compression device 10 and the inner container 8 can be engaged / removed by detachable engaging means (not shown). The engaging means is a normal engaging means such as a hook. When the solid precipitate 12 is taken out of the electrolytic cell 2, the compression device 10 and the inner container 8 are engaged by the engaging means, and the solid precipitate 12 is pulled up from the liquid metal cathode 6 together with the inner container 8. The solid precipitate 12 is recovered. Thereby, the solid deposit 12 can be recovered without stopping the operation of the electrolytic cell 2. When the inner container 8 is pulled up, the liquid metal in the inner container 8 is returned to the cathode crucible through a filter 8a made of a mesh or sintered metal provided at the lower part of the inner container 8, and can be used again as a cathode. It becomes.

本第３の実施の形態によれば、内側容器８の底部に圧縮された固体析出物１２を、適宜、電解槽２の外部に取り出すことにより、良好な回収効率を維持することができ、陰極ルツボ７のサイズや装荷する液体金属量を増加することなく、より多くのＵ、ＴＲＵを効率的に回収することが可能となる。   According to the third embodiment, the solid deposit 12 compressed at the bottom of the inner container 8 can be appropriately taken out of the electrolytic cell 2 to maintain good recovery efficiency, and the cathode More U and TRU can be efficiently recovered without increasing the size of the crucible 7 or the amount of liquid metal to be loaded.

（第４の実施の形態）
第４の実施の形態を図５を用いて説明する。
固形析出物１２は上述した第１、第２及び第３の実施の形態で示した操作を繰り返すことにより圧縮、回収されるが、電解精製が進行するにつれ液体金属陰極ルツボ７内の液体金属はルツボ外容器９にあふれ出るため液位が低下する。この液位を回復するため液体陰極材導入管１３を設置し、ここから液体金属材料１４を導入することで液体金属陰極の液位を回復する。 (Fourth embodiment)
A fourth embodiment will be described with reference to FIG.
The solid precipitate 12 is compressed and recovered by repeating the operations shown in the first, second, and third embodiments. However, as the electrolytic purification proceeds, the liquid metal in the liquid metal cathode crucible 7 is The liquid level drops because the container 9 overflows from the crucible. In order to recover the liquid level, a liquid cathode material introducing tube 13 is installed, and the liquid metal material 14 is introduced from the liquid cathode material introducing tube 13 to recover the liquid level of the liquid metal cathode.

本第４の実施の形態によれば、電気炉１を停止することなく液体金属材料を補充することで、液体金属陰極の液位を適正に保ち、定常的に液体陰極をＵ、ＴＲＵ同時回収及び電解可能な状態に維持することが出来る。   According to the fourth embodiment, by replenishing the liquid metal material without stopping the electric furnace 1, the liquid metal cathode is kept at an appropriate liquid level, and the liquid cathode is regularly recovered simultaneously with U and TRU. And can be maintained in an electrolysable state.

（第５の実施の形態）
第５の実施の形態を図６を用いて説明する。
上述した第１、第２、第３及び第４の実施の形態で説明した操作を繰り返すことにより、固体析出物の圧縮、回収及び液位の回復を行うが、電解精製が進行するにつれ液体金属陰極ルツボ７からあふれ出したＵ、ＴＲＵの溶解した液体金属はルツボ外容器９に溜まっていく。そこで液体金属はルツボ外容器９に溜まった液体金属の液面がある程度上昇したら、液体金属吸い出し管１５をルツボ外容器９内に挿入し、液体金属吸い出し管１５の逆の端部を減圧ポンプまたは減圧容器１６に接続することで、ルツボ外容器９内の液体金属を電解槽外に回収する。 (Fifth embodiment)
A fifth embodiment will be described with reference to FIG.
By repeating the operations described in the first, second, third, and fourth embodiments, the solid precipitate is compressed, recovered, and the liquid level is recovered. As the electrolytic purification proceeds, the liquid metal The liquid metal in which U and TRU overflowing from the cathode crucible 7 is dissolved in the crucible outer container 9. Therefore, when the level of the liquid metal accumulated in the crucible outer container 9 rises to some extent, the liquid metal sucking pipe 15 is inserted into the crucible outer container 9 and the opposite end of the liquid metal sucking pipe 15 is connected to the decompression pump or By connecting to the decompression container 16, the liquid metal in the crucible outer container 9 is recovered outside the electrolytic cell.

本第５の実施の形態によれば、電気炉１を停止することなくルツボ外容器９に貯留されたＵ、ＴＲＵ溶解液体陰極を回収することができる。
なお、本発明に用いられ液体金属陰極６は、低融点の金属であれば、カドミウム、亜鉛、鉛、錫、マグネシウム、ビスマスおよびこれらの金属の混合物が使用可能である。 According to the fifth embodiment, the U and TRU dissolved liquid cathodes stored in the outer crucible container 9 can be recovered without stopping the electric furnace 1.
As the liquid metal cathode 6 used in the present invention, cadmium, zinc, lead, tin, magnesium, bismuth and a mixture of these metals can be used as long as they are low melting point metals.

本発明の第１の実施の形態に係る溶融塩電解精製装置の全体構成図。BRIEF DESCRIPTION OF THE DRAWINGS The whole block diagram of the molten salt electrorefining apparatus which concerns on the 1st Embodiment of this invention. 図２（ａ）、（ｂ）は本発明の第１の実施の形態に係る圧縮装置の挿入及び引き上げ状態を示す図。FIGS. 2A and 2B are views showing insertion and pulling states of the compression device according to the first embodiment of the present invention. 本発明の第２の実施の形態に係る液体金属陰極及び圧縮装置の構成図。The block diagram of the liquid metal cathode and compression apparatus which concern on the 2nd Embodiment of this invention. 本発明の第３の実施の形態に係る液体金属陰極及び圧縮装置の構成図。The block diagram of the liquid metal cathode and compression apparatus which concern on the 3rd Embodiment of this invention. 本発明の第４の実施の形態に係る溶融塩電解精製装置の全体構成図。The whole block diagram of the molten salt electrorefining apparatus which concerns on the 4th Embodiment of this invention. 本発明の第５の実施の形態に係る液体金属陰極及び圧縮装置の構成図。The block diagram of the liquid metal cathode and compression apparatus which concern on the 5th Embodiment of this invention.

符号の説明Explanation of symbols

１…電気炉、２…電解槽、３…溶融塩、４…使用済み核燃料、５…陽極容器、６…液体金属陰極、７…液体金属陰極ルツボ、８…内側容器、８ａ…フィルター、９…ルツボ外容器、１０…圧縮装置、１０ａ…フィルター、１１…電源、１２…固体析出物、１３…液体陰極材導入管、１４…液体金属材料、１５…液体金属吸い出し管、１６…ポンプ又は減圧容器。   DESCRIPTION OF SYMBOLS 1 ... Electric furnace, 2 ... Electrolysis cell, 3 ... Molten salt, 4 ... Used nuclear fuel, 5 ... Anode container, 6 ... Liquid metal cathode, 7 ... Liquid metal cathode crucible, 8 ... Inner container, 8a ... Filter, 9 ... Crucible outer container, 10 ... compressor, 10a ... filter, 11 ... power source, 12 ... solid precipitate, 13 ... liquid cathode material introduction tube, 14 ... liquid metal material, 15 ... liquid metal suction tube, 16 ... pump or vacuum vessel .

Claims (11)

溶融塩が収容された電解槽と、使用済み核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する溶融塩電解精製装置において、前記液体金属陰極の界面に発生する固体析出物を液体金属陰極底部に圧縮する昇降可能な圧縮装置を備えたことを特徴とする溶融塩電解精製装置。   In a molten salt electrorefining apparatus having an electrolytic cell containing a molten salt, an anode container loaded with spent nuclear fuel, and a liquid metal crucible containing a liquid metal cathode, the liquid metal cathode is generated at the interface. A molten salt electrorefining apparatus comprising a compression device capable of moving up and down to compress a solid precipitate to be compressed into the bottom of a liquid metal cathode. 溶融塩が収容された電解槽と、使用済み核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する溶融塩電解精製装置において、前記液体金属陰極の界面に発生する固体析出物を液体金属陰極底部に圧縮する昇降可能な圧縮装置と、前記液体金属ルツボの内側に設けられた内側容器と、を備えたことを特徴とする溶融塩電解精製装置。   In a molten salt electrorefining apparatus having an electrolytic cell containing a molten salt, an anode container loaded with spent nuclear fuel, and a liquid metal crucible containing a liquid metal cathode, the liquid metal cathode is generated at the interface. A molten salt electrorefining apparatus comprising: a compression device capable of moving up and down to compress a solid precipitate to be compressed into a liquid metal cathode bottom portion; and an inner container provided inside the liquid metal crucible. 前記圧縮装置の下部にメッシュまたは焼結金属等からなるフィルターが設けられていることを特徴とする請求項１又は２記載の溶融塩電解精製装置。   The molten salt electrolytic purification apparatus according to claim 1 or 2, wherein a filter made of mesh or sintered metal is provided at a lower portion of the compression apparatus. 前記内側容器の下部にメッシュまたは焼結金属等からなるフィルターが設けられていることを特徴とする請求項２又は３いずれか１項記載の溶融塩電解精製装置。   The molten salt electrolytic purification apparatus according to any one of claims 2 and 3, wherein a filter made of mesh or sintered metal is provided at a lower portion of the inner container. 液体金属陰極ルツボに液体金属陰極材料を供給する液体金属陰極材料供給管を設けたことを特徴とする請求項１乃至４いずれか１項記載の溶融塩電解精製装置。   5. The molten salt electrorefining apparatus according to claim 1, further comprising a liquid metal cathode material supply pipe for supplying the liquid metal cathode material to the liquid metal cathode crucible. 前記圧縮装置と前記内側容器とを着脱可能に係合する係合手段を設けたことを特徴とする請求項２乃至５いずれか１項記載の溶融塩電解精製装置。   The molten salt electrolytic purification apparatus according to any one of claims 2 to 5, further comprising engagement means for detachably engaging the compression apparatus and the inner container. 前記液体金属陰極ルツボの外側にルツボ外容器を設けたことを特徴とする請求項１乃至６いずれか１項記載の溶融塩電解精製装置。   The molten salt electrorefining apparatus according to claim 1, wherein a crucible outer container is provided outside the liquid metal cathode crucible. 前記ルツボ外容器に前記ルツボ外容器内の液体金属を吸い出す吸い出し管を設けたことを特徴とする請求項７記載の溶融塩電解精製装置。   8. The molten salt electrolytic purification apparatus according to claim 7, wherein a suction pipe for sucking out the liquid metal in the outer crucible container is provided in the outer crucible container. 前記液体金属陰極がカドミウム、亜鉛、鉛、錫、マグネシウム、ビスマス又はこれらの金属の混合物からなることを特徴とする請求項１乃至８いずれか１項記載の溶融塩電解精製装置。   9. The molten salt electrorefining apparatus according to claim 1, wherein the liquid metal cathode is made of cadmium, zinc, lead, tin, magnesium, bismuth or a mixture of these metals. 溶融塩が収容された電解槽と、使用済み核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する使用済み核燃料の溶融塩電解精製方法において、下部にメッシュまたは焼結金属等からなるフィルターが設けられた圧縮装置を液体金属陰極内に下降させ、前記液体金属陰極の界面に発生する固体析出物を前記液体金属陰極底部に圧縮することを特徴とする溶融塩電解精製方法。   In a molten salt electrorefining method for spent nuclear fuel, comprising: an electrolytic cell containing a molten salt; an anode container loaded with a spent nuclear fuel; and a liquid metal crucible containing a liquid metal cathode. A molten salt characterized by lowering a compression apparatus provided with a filter made of sintered metal or the like into a liquid metal cathode and compressing solid precipitates generated at the interface of the liquid metal cathode to the bottom of the liquid metal cathode Electrolytic purification method. 溶融塩が収容された電解槽と、使用済み核燃料が装荷された陽極容器と、液体金属陰極が収容された液体金属ルツボと、を有する使用済み核燃料の溶融塩電解精製方法において、下部にメッシュまたは焼結金属等からなるフィルターが設けられた圧縮装置を前記液体金属陰極内に下降させ、前記圧縮装置と前記液体金属ルツボの内側に設けられた内側容器とを係合し、前記圧縮装置と前記内側容器を係合させた状態で前記圧縮装置を引き上げることを特徴とする溶融塩電解精製方法。   In a molten salt electrorefining method for spent nuclear fuel, comprising: an electrolytic cell containing a molten salt; an anode container loaded with a spent nuclear fuel; and a liquid metal crucible containing a liquid metal cathode. A compression device provided with a filter made of sintered metal or the like is lowered into the liquid metal cathode, the compression device and an inner container provided inside the liquid metal crucible are engaged, and the compression device and the A molten salt electrolytic purification method, wherein the compression device is pulled up with the inner container engaged.
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