JP2000355784A - Oxidation decomposition apparatus of organic solvent and oxidation decomposition method therefor - Google Patents
Oxidation decomposition apparatus of organic solvent and oxidation decomposition method thereforInfo
- Publication number
- JP2000355784A JP2000355784A JP11169440A JP16944099A JP2000355784A JP 2000355784 A JP2000355784 A JP 2000355784A JP 11169440 A JP11169440 A JP 11169440A JP 16944099 A JP16944099 A JP 16944099A JP 2000355784 A JP2000355784 A JP 2000355784A
- Authority
- JP
- Japan
- Prior art keywords
- organic solvent
- chamber
- electrolytic
- electrolytic solution
- electrolyte
- 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.)
- Withdrawn
Links
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、水に不混和で水よ
り比重の小さい有機溶媒を電気化学的手法によって酸化
分解処理する装置及びその方法に関するものである。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an apparatus and method for oxidatively decomposing an organic solvent immiscible with water and having a lower specific gravity than water by an electrochemical method.
【０００２】[0002]
【従来の技術】水に混和する溶媒を電気化学的手法によ
って酸化分解する方法として、銀イオン等の電解酸化に
よって強力な酸化種として機能するレドックス種を含有
する硝酸を主成分とする水性電解液に電位差を与えてそ
のレドックス種を酸化種として機能させ、この電解液に
溶媒を混合する方法が知られている（特開平１−３０６
８９）。この方法では、銀の２価イオンにより溶媒が分
解され、分解に寄与して１価イオンに変化した銀イオン
は水性電解液に与えられる電位差により再び２価イオン
に変化して再生され、再び分解に寄与するようになって
いる。しかし、この酸化分解方法を水と混和することの
ない有機溶媒の分解に使用すると、分解反応が有機溶媒
と電解液の界面で行われることになるため、水に混和す
る溶媒を分解する場合に比較して分解速度が遅くなる不
具合がある。また、生成した酸化種の多くが瞬時に消費
されず、それらの電解液中における濃度が増加する結
果、生成した酸化種の内の水との分解反応によって消費
される割合を増加させ酸化分解処理に対する電気的効率
の低下を招く不具合もある。この点を解消するために
は、電解液と溶媒とを流通させて生成した酸化種を直ち
に分解処理によって消費させることが求められる。2. Description of the Related Art As a method of oxidatively decomposing a solvent miscible with water by an electrochemical method, an aqueous electrolyte mainly containing nitric acid containing a redox species which functions as a strong oxidizing species by electrolytic oxidation of silver ions or the like is used. A method is known in which a redox species is made to function as an oxidizing species by giving a potential difference to the electrolyte, and a solvent is mixed with the electrolytic solution (JP-A-1-306).
89). In this method, the solvent is decomposed by divalent silver ions, and the silver ions that have been converted to monovalent ions by contributing to the decomposition are converted into divalent ions again by the potential difference applied to the aqueous electrolyte, and are regenerated. It has become to contribute to. However, if this oxidative decomposition method is used to decompose an organic solvent that is not miscible with water, the decomposition reaction will take place at the interface between the organic solvent and the electrolytic solution. There is a problem that the decomposition speed is slower than that. In addition, most of the generated oxidizing species are not consumed instantaneously, and their concentration in the electrolytic solution increases. As a result, the ratio of the generated oxidizing species consumed by the decomposition reaction with water increases, and the oxidative decomposition treatment increases. There is also a problem that leads to a decrease in electrical efficiency with respect to. In order to solve this problem, it is required that the oxidized species generated by flowing the electrolytic solution and the solvent be immediately consumed by the decomposition treatment.
【０００３】このための装置として有機溶媒と電解液を
循環させる手段を備えた電気化学セルが提案されている
（特表平４−５０４３０３）。この電気化学セルにおけ
る循環手段は、有機溶媒と電解液を貯留する槽の略中央
部に、周囲に複数の孔が形成され内部に複数の翼が設け
られた回転体を設けたドラフト管を鉛直に挿入したもの
である。複数の翼は回転体とともに回転して周囲の孔か
らドラフト管内部に侵入した有機溶媒及び電解液を下方
に向って押出すように構成される。一方、上述の電気化
学セルでは複数の球体からなる電極を層状にその槽の下
部に配設し、翼の回転によりドラフト管の下部開口部か
ら槽の下部に排出された有機溶媒及び電解液は、電極で
ある複数の球体の間を下方から上方に通過するように構
成される。この電気化学セルでは、複数の球体の間を通
過する際に銀の１価イオンは酸化種として機能する２価
イオンに変化し、その層状の電極を通過した酸化種は直
ちに有機溶媒の分解処理に寄与することができるように
なっている。As an apparatus for this purpose, there has been proposed an electrochemical cell provided with means for circulating an organic solvent and an electrolyte (Japanese Patent Application Laid-Open No. 4-504303). The circulating means in this electrochemical cell is a vertical pipe provided with a rotating body having a plurality of holes formed therein and a plurality of wings provided in a substantially central portion of a tank for storing an organic solvent and an electrolytic solution. It is inserted in. The plurality of blades are configured to rotate together with the rotating body to push out the organic solvent and the electrolyte that have entered the inside of the draft tube from the surrounding holes downward. On the other hand, in the above-mentioned electrochemical cell, electrodes composed of a plurality of spheres are arranged in layers at the lower part of the tank, and the organic solvent and the electrolyte discharged from the lower opening of the draft tube to the lower part of the tank by the rotation of the wings are Is configured to pass between a plurality of spheres, which are electrodes, from above to below. In this electrochemical cell, when passing between a plurality of spheres, the monovalent ions of silver are changed to divalent ions that function as oxidizing species, and the oxidizing species passing through the layered electrode are immediately subjected to a decomposition treatment of an organic solvent. Can be contributed to.
【０００４】[0004]
【発明が解決しようとする課題】しかし、上述した電気
化学セルでは循環手段を設けている他に、複数の球体か
らなる電極を層状に槽の下部に配設する必要があり、セ
ル自体の構造が複雑になる不具合がある。また、上述し
た電気化学セルでは、陽極室を構成する多孔性ポットの
内部に循環手段及び層状の電極を設けているが、高腐食
性雰囲気下におかれる陽極室内においては、材料として
耐食性に強くかつ高価なチタン等を使用する必要があ
る。このため、上述した電気化学セルは極めて高価にな
る不具合がある。特に、この多孔性ポット自体も規模が
大きくなるに従って高価になるものになるため、多孔性
ポットを使用して構成することができる電気化学セルの
大きさには一定の限度がある。更に、上述した電気化学
セルでは、廃棄物を連続的に処理する場合には、別にこ
の廃棄物を処理速度に応じて供給する装置が必要になる
不具合もある。本発明の目的は、有機溶媒と電解液の界
面面積を十分に増大し、かつ電解液の電解酸化で生成し
た酸化種の有機溶媒との接触時間を確保して分解の電気
効率を十分に速めることができ、かつ有機溶媒の連続処
理を容易に行える簡単な構造の有機溶媒の酸化分解装置
及びその酸化分解方法を提供することにある。However, in the above-mentioned electrochemical cell, in addition to the provision of the circulation means, it is necessary to arrange a plurality of spherical electrodes at the bottom of the tank in a layered manner. Is complicated. Further, in the above-described electrochemical cell, the circulation means and the layered electrodes are provided inside the porous pot constituting the anode chamber. However, in the anode chamber placed under a highly corrosive atmosphere, the material has a strong corrosion resistance as a material. In addition, it is necessary to use expensive titanium or the like. For this reason, there is a problem that the above-mentioned electrochemical cell becomes extremely expensive. In particular, the size of an electrochemical cell that can be configured using a porous pot has a certain limit, because the porous pot itself becomes more expensive as the scale increases. Further, in the above-described electrochemical cell, when waste is continuously processed, there is a problem that a device for separately supplying the waste according to a processing speed is required. An object of the present invention is to sufficiently increase the interfacial area between an organic solvent and an electrolytic solution, and to sufficiently increase the electrical efficiency of decomposition by securing the contact time of the oxidizing species generated by electrolytic oxidation of the electrolytic solution with the organic solvent. It is an object of the present invention to provide an organic solvent oxidative decomposition apparatus and a method for oxidative decomposition of the organic solvent having a simple structure capable of easily performing a continuous treatment of the organic solvent.
【０００５】[0005]
【課題を解決するための手段】請求項１に係る発明は、
図１に示すように、オキソ酸を主成分とし電解酸化によ
って強力な酸化種として機能するレドックス種を含む水
性電解液１１を貯え電解液中に配置された陽極１２ａと
陰極１２ｂとの間に電位差を与えることによりレドック
ス種を酸化種として機能させる電解槽１２と、酸化種を
含む電解液１１と水に不混和で水より比重の小さい有機
溶媒１３とを撹拌手段１４により混合して有機溶媒１３
を酸化分解するミキサ室１６ａと、ミキサ室１６ａに隔
壁１６ｂを隔てて隣接され隔壁１６ｂを越えて溢れた未
分解の有機溶媒１３及び電解液１１を静置することによ
り互いに分離するセトラ室１６ｃとを有する反応槽１６
とを備え、撹拌手段１４の撹拌により反応槽１６で使用
した電解液１１を電解槽１２に導きかつ電解槽１２の電
解液１１を反応槽１６に導くように構成された有機溶媒
の酸化分解装置である。The invention according to claim 1 is
As shown in FIG. 1, a potential difference between an anode 12a and a cathode 12b, which contain an aqueous electrolyte solution 11 containing oxo acid as a main component and containing a redox species which functions as a strong oxidizing species by electrolytic oxidation and is disposed in the electrolyte solution. And the electrolytic solution 11 containing the oxidizing species and the organic solvent 13 immiscible with water and having a lower specific gravity than water are mixed by the stirring means 14 to form the organic solvent 13.
Chamber 16a that oxidatively decomposes the organic solvent 13 and a settling chamber 16c that is adjacent to the mixer chamber 16a with the partition 16b interposed therebetween and separates the undecomposed organic solvent 13 and the electrolyte 11 that have overflowed beyond the partition 16b. Reaction tank 16 having
An organic solvent oxidative decomposition device configured to guide the electrolytic solution 11 used in the reaction vessel 16 to the electrolytic vessel 12 and to guide the electrolytic solution 11 in the electrolytic vessel 12 to the reaction vessel 16 by stirring of the stirring means 14. It is.
【０００６】オキソ酸としては、硫酸（Ｈ2ＳＯ4）又は
硝酸（ＨＮＯ3）が例示され、レドックス種としては１
価の銀イオン，２価のコバルトイオン又は３価のセリウ
ムイオンが例示される。なお、これらは電解酸化によっ
て強力な酸化種である２価の銀イオン，３価のコバルト
イオン又は４価のセリウムイオンになる。分解の対象で
ある有機溶媒としては、原子力の分野で発生するもの及
び一般工業分野におけるものの双方が挙げられる。原子
力の分野で発生するものとしては放射性物質を含む廃棄
物として発生するドデカン、ＴＢＰ(tributyl phosphat
e)、デカリン、ＣＭＰＯ(carbamoylmethylphosphine ox
ide)、トルエン、ケロシン、ポンプ油、又はシンチレー
タカクテルが挙げられ、シンチレータカクテルに含まれ
る有機溶媒としてはキシレン、デカリン、シェルゾール
Ａ、ターフェニル、トリエチルベンゼン、フェニルシク
ロヘキサンが挙げられる。一般工業分野におけるものと
しては、シクロヘキサン等のシクロアルカン類、メチル
エーテル等のエーテル類、エチルベンゼン等のベンゼン
類、多価のアルコールを除く高級アルコール類が挙げら
れる。Examples of oxo acids include sulfuric acid (H 2 SO 4 ) and nitric acid (HNO 3 ).
A valent silver ion, a divalent cobalt ion or a trivalent cerium ion is exemplified. These are converted into strong oxidizing species such as divalent silver ions, trivalent cobalt ions or tetravalent cerium ions by electrolytic oxidation. Organic solvents to be decomposed include those generated in the field of nuclear power and those in the general industrial field. In the field of nuclear power, dodecane and TBP (tributyl phosphat) generated as waste containing radioactive materials
e), decalin, CMPO (carbamoylmethylphosphine ox)
ide), toluene, kerosene, pump oil, or a scintillator cocktail. Examples of the organic solvent contained in the scintillator cocktail include xylene, decalin, Shersol A, terphenyl, triethylbenzene, and phenylcyclohexane. Examples in the general industrial field include cycloalkanes such as cyclohexane, ethers such as methyl ether, benzenes such as ethylbenzene, and higher alcohols excluding polyhydric alcohols.
【０００７】なお、この明細書において「有機溶媒」と
は上述したもの単体の他に上述のものに被酸化性物質が
溶解されたものも含む。溶解される被酸化性物質には、
二酸化ウラン、二酸化プルトニウム等の核燃料物質、工
場の操業プロセスで混入した金属、金属酸化物、又は固
形有機物が挙げられ、固形有機物には濾紙、キムワイ
プ、キムタオル、マウス等の生物試料、活性炭等が含ま
れる。この請求項１に係る発明では、電解液１１と有機
溶媒１３とを撹拌手段１４により混合するので、有機溶
媒と電解液の界面面積を増大することができ、撹拌手段
１４の撹拌により電解槽１２の電解液１１は反応槽１６
に導かれるので、電解槽１２で生成された酸化種は反応
槽１６で直ちに有機溶媒の分解処理に寄与する。また、
反応槽１６が有機溶媒１３及び電解液１１を分離するセ
トラ室１６ｃを有するので、反応槽１６で使用した電解
液１１のみが撹拌手段１４の撹拌により電解槽１２に導
かれる。[0007] In this specification, the term "organic solvent" includes not only the above-mentioned substances but also those in which an oxidizable substance is dissolved in the above-mentioned substances. The dissolved oxidizable substances include:
Examples include nuclear fuel materials such as uranium dioxide and plutonium dioxide, metals, metal oxides, or solid organic matter mixed in the operation processes of factories. It is. According to the first aspect of the present invention, since the electrolytic solution 11 and the organic solvent 13 are mixed by the stirring means 14, the interface area between the organic solvent and the electrolytic solution can be increased. Of the electrolytic solution 11 in the reaction tank 16
The oxidized species generated in the electrolytic cell 12 immediately contributes to the decomposition treatment of the organic solvent in the reaction tank 16. Also,
Since the reaction tank 16 has a settling chamber 16 c for separating the organic solvent 13 and the electrolyte 11, only the electrolyte 11 used in the reaction tank 16 is guided to the electrolysis tank 12 by the stirring of the stirring means 14.
【０００８】請求項２に係る発明は、請求項１に係る発
明であって、酸化分解される有機溶媒１３を貯えかつセ
トラ室１６ｃで分離された未分解の有機溶媒１３が流入
可能に構成された溶媒槽１７と、溶媒槽１７に貯えられ
た有機溶媒１３をミキサ室に導くポンプ１７ｄとを更に
備えた有機溶媒の酸化分解装置である。この請求項２に
係る発明では、溶媒槽１７を独立して設けることにより
被酸化性物質を溶媒１３に溶解させることが容易にな
り、この溶媒槽１７をセトラ室１６ｃにおける未分解の
有機溶媒１３が流入可能に構成することにより反応槽１
６における有機溶媒１３と電解液１１からなる液面を常
に一定に保つことができる。The invention according to claim 2 is the invention according to claim 1, wherein the organic solvent 13 to be oxidatively decomposed is stored, and the undecomposed organic solvent 13 separated in the settling chamber 16c is allowed to flow therein. This is an organic solvent oxidative decomposition apparatus further comprising a solvent tank 17 and a pump 17d for guiding the organic solvent 13 stored in the solvent tank 17 to the mixer chamber. According to the second aspect of the present invention, it is easy to dissolve the oxidizable substance in the solvent 13 by providing the solvent tank 17 independently. To allow the reaction vessel 1 to flow
The liquid surface composed of the organic solvent 13 and the electrolytic solution 11 in 6 can always be kept constant.
【０００９】請求項３に係る発明は、請求項１又は２に
係る発明であって、撹拌手段１４が、ミキサ室１６ａ上
方に設けられた電動モータ１４ａと、ミキサ室１６ａ内
に鉛直に設けられ下端がミキサ室１６ａの下部に達し上
端が電動モータ１４ａの回転軸に連結された回転軸１４
ｂと、回転軸１４ｂの下端に設けられ回転軸１４ｂとと
もに回転して電解液１１及び有機溶媒１３を混合可能に
構成された回転翼１４ｃとを有し、セトラ室１６ｃの下
部と電解槽１２が第１配管１８により連結され、電解槽
１２と回転翼１４ｃに臨むミキサ室１６ａの下部とが第
２配管１９により連結され、回転翼１４ｃの回転により
第２配管１９を介して電解槽１２の電解液１１をミキサ
室１６ａに導きかつ第１配管１８を介してセトラ室１６
ｃの電解液１１を電解槽１２に導くように構成された有
機溶媒の酸化分解装置である。この請求項３に係る発明
では、回転翼１４ｃの回転により電解槽１２の電解液１
１をミキサ室１６ａに導きかつセトラ室１６ｃの電解液
１１を電解槽１２に導くので、電解液１１を循環させる
ための特別の装置を不要にして装置自体を簡素化させ
る。The invention according to claim 3 is the invention according to claim 1 or 2, wherein the stirring means 14 is provided vertically with the electric motor 14a provided above the mixer chamber 16a and inside the mixer chamber 16a. A rotating shaft 14 whose lower end reaches the lower portion of the mixer chamber 16a and whose upper end is connected to the rotating shaft of the electric motor 14a.
b, and rotating blades 14c provided at the lower end of the rotating shaft 14b and configured to rotate together with the rotating shaft 14b so as to be able to mix the electrolytic solution 11 and the organic solvent 13; The electrolytic cell 12 is connected to the lower part of the mixer chamber 16a facing the rotary blade 14c by a first pipe 18, and the lower part of the mixer chamber 16a is connected by a second pipe 19, and the electrolytic cell 12 is electrolyzed through the second pipe 19 by the rotation of the rotary blade 14c. The liquid 11 is introduced into the mixer chamber 16 a and settled through the first pipe 18.
This is an organic solvent oxidative decomposition device configured to guide the electrolytic solution 11c to the electrolytic cell 12. In the invention according to the third aspect, the rotation of the rotary blade 14c causes the electrolyte 1 in the electrolytic cell 12 to rotate.
1 is introduced into the mixer chamber 16a and the electrolyte 11 in the settle chamber 16c is introduced into the electrolytic cell 12, so that a special device for circulating the electrolyte 11 is not required and the device itself is simplified.
【００１０】請求項４に係る発明は、電解槽１２でオキ
ソ酸を主成分とし電解酸化によって強力な酸化種として
機能するレドックス種を含む水性電解液１１を電解して
レドックス種を酸化種として機能させる工程と、ミキサ
室１６ａに水に不混和で水より比重の小さい有機溶媒１
３を導入する工程と、電解槽１２の酸化種を含む電解液
１１をミキサ室１６ａに導入して有機溶媒１３と混合す
ることにより有機溶媒１３を酸化分解する工程と、ミキ
サ室１６ａで未分解の有機溶媒１３と電解液１１をセト
ラ室１６ｃで静置して互いに分離する工程と、セトラ室
１６ｃで分離した電解液１１を電解槽１２に戻す工程
と、セトラ室１６ｃで分離した未分解の有機溶媒１３を
再びミキサ室１６ａに導入する工程とを含む有機溶媒の
酸化分解方法である。この請求項４に係る発明では、有
機溶媒１３が常に循環しているので、いわゆるバッチ処
理及び連続処理の双方において使用することができ、従
来必要とされた処理時間を考慮して有機溶媒１３を投入
する手間を省くことができる。また、比較的多くの有機
溶媒１３を投入した場合にあってもその有機溶媒１３が
反応槽１６から溢れることはなく、比較的多くの有機溶
媒の同時処理が可能になる。[0010] The invention according to claim 4 is an electrolysis cell in which an aqueous electrolyte solution 11 containing oxo acid as a main component and containing a redox species which functions as a strong oxidizing species by electrolytic oxidation is electrolyzed, and the redox species functions as an oxidizing species. And an organic solvent 1 immiscible with water and having a specific gravity lower than that of water in the mixer chamber 16a.
3, the step of introducing the electrolytic solution 11 containing the oxidizing species in the electrolytic cell 12 into the mixer chamber 16a and mixing it with the organic solvent 13 to oxidatively decompose the organic solvent 13, and the step of undecomposing the organic solvent 13 in the mixer chamber 16a. Leaving the organic solvent 13 and the electrolyte solution 11 in a settling chamber 16c to separate them from each other, returning the electrolyte solution 11 separated in the settling chamber 16c to the electrolytic bath 12, And introducing the organic solvent 13 into the mixer chamber 16a again. In the invention according to claim 4, since the organic solvent 13 is constantly circulated, it can be used in both so-called batch processing and continuous processing, and the organic solvent 13 can be used in consideration of the processing time conventionally required. It is possible to save the trouble of inputting. Further, even when a relatively large amount of the organic solvent 13 is supplied, the organic solvent 13 does not overflow from the reaction tank 16, and a relatively large number of the organic solvents can be simultaneously processed.
【００１１】[0011]
【発明の実施の形態】次に本発明の実施の形態を図面に
基づいて詳しく説明する。図１に示すように、有機溶媒
の酸化分解装置１０は、水性電解液１１を貯える電解槽
１２と、その電解液１１と有機溶媒１３とを撹拌手段１
４により混合する反応槽１６と、酸化分解される有機溶
媒１３を貯える溶媒槽１７とを備える。水性電解液１１
は硫酸（Ｈ2ＳＯ4）又は硝酸（ＨＮＯ3）等のオキソ酸
を主成分とし、１価の銀イオン，２価のコバルトイオン
又は３価のセリウムイオン等の電解酸化によって強力な
酸化種として機能するレドックス種を含むものである。
この実施の形態における電解槽１２は円筒状の有底容器
であり、白金により構成され電解液１１中に配置される
陽極１２ａと陰極１２ｂを備える。陰極１２ｂはその容
器の中央に鉛直方向に延びて設けられた棒状部材であ
り、その陰極１２ｂの周囲には円筒状の多孔質の絶縁性
隔壁１２ｃが同心状に設けられる。なお、陰極１２ｂは
オキソ酸に耐え得るものであればステンレス鋼その他の
鋼材であっても良い。Embodiments of the present invention will now be described in detail with reference to the drawings. As shown in FIG. 1, an organic solvent oxidative decomposition device 10 includes an electrolytic tank 12 for storing an aqueous electrolytic solution 11 and a stirring means 1 for mixing the electrolytic solution 11 and the organic solvent 13.
4 and a solvent tank 17 for storing an organic solvent 13 to be oxidatively decomposed. Aqueous electrolyte 11
Is mainly composed of oxoacids such as sulfuric acid (H 2 SO 4 ) or nitric acid (HNO 3 ), and is a strong oxidizing species by electrolytic oxidation of monovalent silver ion, divalent cobalt ion or trivalent cerium ion. Includes functional redox species.
The electrolytic cell 12 in this embodiment is a cylindrical bottomed container, and includes an anode 12a and a cathode 12b made of platinum and arranged in the electrolytic solution 11. The cathode 12b is a rod-shaped member provided in the center of the container so as to extend in the vertical direction, and a cylindrical porous insulating partition 12c is provided concentrically around the cathode 12b. The cathode 12b may be stainless steel or another steel material as long as it can withstand oxoacid.
【００１２】陽極１２ａはその隔壁を包囲するように設
けられた網状の筒部材であり、電解液１１が流通可能に
構成される。この電解液１１中に配置された陽極１２ａ
と陰極１２ｂとの間に電位差を与えることにより、電解
槽１２は上述したレドックス種を２価の銀イオン，３価
のコバルトイオン又は４価のセリウムイオン等の酸化種
に変化させるように構成される。また、電解槽１２には
磁性部材１２ｄが底部に挿入され、電解槽の下方には磁
力によりこの磁性部材を回転させる回転装置１２ｅが設
けられる。陽極１２ａと陰極１２ｂとの間に電位差を与
える際に回転装置１２ｅは磁力により磁性部材１２ｄを
電解槽１２の内部で回転させ、電解槽１２内部の電解液
１１を網状の陽極１２ａに強制的に通過させて、レドッ
クス種を有効に酸化種に変化させるように構成される。The anode 12a is a net-like cylindrical member provided so as to surround the partition wall, and is configured so that the electrolyte solution 11 can flow therethrough. Anode 12a arranged in this electrolytic solution 11
By giving a potential difference between the redox species and the cathode 12b, the electrolytic cell 12 is configured to change the above-mentioned redox species into oxidizing species such as divalent silver ions, trivalent cobalt ions or tetravalent cerium ions. You. A magnetic member 12d is inserted into the bottom of the electrolytic bath 12, and a rotating device 12e for rotating the magnetic member by magnetic force is provided below the electrolytic bath. When a potential difference is applied between the anode 12a and the cathode 12b, the rotating device 12e rotates the magnetic member 12d inside the electrolytic bath 12 by magnetic force, and forcibly transfers the electrolytic solution 11 inside the electrolytic bath 12 to the mesh anode 12a. Is configured to pass through and effectively convert redox species to oxidized species.
【００１３】反応槽１６はミキサ室１６ａとこのミキサ
室１６ａに隔壁１６ｂを隔てて隣接されたセトラ室１６
ｃとを備える。ミキサ室１６ａには酸化種を含む水性電
解液１１と水に不混和で水より比重の小さい有機溶媒１
３とを混合して有機溶媒１３を酸化分解する撹拌手段１
４が設けられ、ミキサ室１６ａ上方にはミキサ室１６ａ
で発生するＣＯ2等を図示しない排ガス系に向って排出
する排出口１６ｅが形成される。この実施の形態におけ
る撹拌手段１４は、ミキサ室１６ａ上方に設けられた電
動モータ１４ａと、ミキサ室１６ａ内に鉛直に設けられ
下端がミキサ室１６ａの下部に達し上端が電動モータ１
４ａの回転軸に連結された回転軸１４ｂと、回転軸１４
ｂの下端に設けられ回転軸１４ｂとともに回転して電解
液１１及び有機溶媒１３を混合可能に構成された回転翼
１４ｃとを有する。ミキサ室１６ａから隔壁１６ｂを越
えて溢れた未分解の有機溶媒１３及び電解液１１はセト
ラ室１６ｃで静置可能に構成され、ミキサ室１６ａ近傍
のセトラ室１６ｃには下端が隙間を有し上部が液面上方
に出現した仕切板１６ｄがそのセトラ室１６ｃを分割す
るように設けられる。ミキサ室１６ａから破線矢印で示
すように隔壁１６ｂを越えて溢れた有機溶媒１３及び電
解液１１は、このセトラ室１６ｃで静置され、水に不混
和で水より比重の小さい有機溶媒１３は上方に移動し電
解液１１は下方に移動して互いに分離されるように構成
される。The reaction tank 16 includes a mixer chamber 16a and a settling chamber 16 adjacent to the mixer chamber 16a with a partition wall 16b interposed therebetween.
c. An aqueous electrolyte 11 containing an oxidizing species and an organic solvent 1 immiscible with water and having a lower specific gravity than water are contained in the mixer chamber 16a.
And stirring means 1 for oxidatively decomposing organic solvent 13 by mixing
4 is provided, and the mixer chamber 16a is provided above the mixer chamber 16a.
In the outlet 16e for discharging towards the exhaust system (not shown) the generated CO 2 or the like is formed. The agitating means 14 in this embodiment includes an electric motor 14a provided above the mixer chamber 16a, a vertically provided lower part of the mixer chamber 16a reaching the lower part of the mixer chamber 16a, and an upper end provided with the electric motor 1a.
A rotation shaft 14b connected to the rotation shaft
and a rotating blade 14c provided at a lower end of the rotating blade 14b and configured to be able to rotate together with the rotating shaft 14b to mix the electrolytic solution 11 and the organic solvent 13. The undecomposed organic solvent 13 and the electrolyte 11 overflowing from the mixer chamber 16a over the partition 16b are configured to be able to stand still in a settling chamber 16c, and the lower end of the settling chamber 16c near the mixer chamber 16a has a gap. Is provided so that the partition plate 16d that appears above the liquid surface divides the settling chamber 16c. The organic solvent 13 and the electrolytic solution 11 overflowing from the mixer chamber 16a over the partition wall 16b as shown by the dashed arrow are allowed to stand still in the settle chamber 16c, and the organic solvent 13 that is immiscible with water and has a lower specific gravity than water rises upward. And the electrolyte 11 moves downward and is separated from each other.
【００１４】溶媒槽１７は反応槽１６と水平な連結管１
７ａで連結され、セトラ室１６ｃで分離された未分解の
有機溶媒１３がその連結管１７ａを介して流入可能に構
成され、上部には有機溶媒１３とともに分解する金属，
金属酸化物又は固形有機物をこの溶媒中に投入するため
の投入口１７ｂが設けられる。溶媒槽１７の下部とミキ
サ室１６ａは溶媒管１７ｃにより連結され、溶媒管１７
ｃには溶媒槽１７に貯えられた有機溶媒１３をミキサ室
１６ａに導くポンプ１７ｄが設けられる。また、セトラ
室１６ｃの下部と電解槽１２の下部とが第１配管１８に
より連結され、電解槽１２の上部と撹拌手段１４である
回転翼１４ｃに臨むミキサ室１６ａの下部とは第２配管
１９により連結される。回転翼１４ｃは回転方向に対し
て傾斜して形成され、回転することにより第２配管１９
を介して電解槽１２の電解液１１をミキサ室１６ａに導
くように構成される。このように電解液１１をミキサ室
１６ａに導くことにより回転翼１４ｃは第１配管１８を
介してセトラ室１６ｃの電解液１１を電解槽１２に導く
ように構成される。The solvent tank 17 is connected to the horizontal connecting pipe 1 with the reaction tank 16.
7a, the undecomposed organic solvent 13 separated in the settler chamber 16c is configured to be able to flow in through the connection pipe 17a, and a metal that decomposes together with the organic solvent 13 is provided on the upper part.
A charging port 17b for charging a metal oxide or a solid organic substance into the solvent is provided. The lower part of the solvent tank 17 and the mixer chamber 16a are connected by a solvent pipe 17c.
A pump 17d for guiding the organic solvent 13 stored in the solvent tank 17 to the mixer chamber 16a is provided in c. Further, the lower part of the settling chamber 16c and the lower part of the electrolytic cell 12 are connected by a first pipe 18, and the upper part of the electrolytic cell 12 and the lower part of the mixer chamber 16a facing the rotary blade 14c as the stirring means 14 are connected to a second pipe 19. Are linked by The rotary wing 14c is formed to be inclined with respect to the rotation direction.
Is configured to guide the electrolytic solution 11 of the electrolytic cell 12 to the mixer chamber 16a via the circulating fluid. By guiding the electrolyte 11 to the mixer chamber 16a in this manner, the rotary blade 14c is configured to guide the electrolyte 11 in the settling chamber 16c to the electrolytic tank 12 via the first pipe 18.
【００１５】このように構成された酸化分解装置による
有機溶媒の酸化分解方法について説明する。先ず、有機
溶媒の酸化分解に際して電解槽１２及び反応槽１６には
所定量の水性電解液１１を貯留しておき、溶媒槽１７に
は分解すべき有機溶媒１３を貯留する。その後陽極１２
ａと陰極１２ｂとの間に電位差を与え、電解槽１２で水
性電解液１１を電解してその電解液に含有されるレドッ
クス種を酸化種として機能させる。そして、ポンプ１７
ｄを駆動して溶媒槽１７に貯えられた有機溶媒１３を所
定量だけ溶媒管１７ｃを介してミキサ室１６ａに導入す
る。A method for oxidatively decomposing an organic solvent by the oxidative decomposition apparatus having the above-described structure will be described. First, at the time of oxidative decomposition of the organic solvent, a predetermined amount of the aqueous electrolytic solution 11 is stored in the electrolytic bath 12 and the reaction bath 16, and the organic solvent 13 to be decomposed is stored in the solvent bath 17. Then anode 12
A potential difference is applied between the electrode a and the cathode 12b, and the aqueous electrolyte 11 is electrolyzed in the electrolytic bath 12 so that the redox species contained in the electrolyte functions as an oxidizing species. And the pump 17
By driving d, a predetermined amount of the organic solvent 13 stored in the solvent tank 17 is introduced into the mixer chamber 16a via the solvent pipe 17c.
【００１６】その後、撹拌手段１４の電動モータ１４ａ
を駆動して回転軸１４ｂとともに回転翼１４ｃを回転さ
せ、ミキサ室１６ａの貯留された電解液１１及び溶媒槽
１７から導入された有機溶媒１３を混合する。回転翼１
４ｃは回転することにより第２配管１９を介して電解槽
１２の電解液１１をミキサ室１６ａに導き、電解槽１２
で変えられた酸化種を含む電解液１１はミキサ室１６ａ
で有機溶媒１３と混合することによりこの有機溶媒１３
を酸化分解する。有機溶媒１３がベンゼンである場合の
分解反応を例示すると、以下（１）の反応式で示すよう
に分解され、この分解時に発生するＣＯ2は排出口１６
ｅから図示しない排ガス系に向って排出される。Thereafter, the electric motor 14a of the stirring means 14
To rotate the rotary blade 14c together with the rotary shaft 14b to mix the electrolytic solution 11 stored in the mixer chamber 16a and the organic solvent 13 introduced from the solvent tank 17. Rotor 1
4c rotates to guide the electrolytic solution 11 in the electrolytic cell 12 to the mixer chamber 16a through the second pipe 19,
The electrolytic solution 11 containing the oxidized species changed in
And the organic solvent 13
Oxidatively decomposes. As an example of the decomposition reaction when the organic solvent 13 is benzene, the decomposition is performed as shown by the following reaction formula (1), and CO 2 generated during the decomposition is discharged to the outlet 16.
e to an exhaust gas system (not shown).
【００１７】 Ｃ6Ｈ6＋４２Ｈ2Ｏ＋３０Ａｇ2+→６ＣＯ2↑＋３０Ｈ3０+＋３０Ａｇ+…（１） 電解槽１２から電解液１１が、溶媒槽１７から有機溶媒
１３が供給されることにより、ミキサ室１６ａからは隔
壁１６ｂを越えて溢れた未分解の有機溶媒１３及び電解
液１１がセトラ室１６ｃに図の破線矢印で示すように流
入する。このように流入した有機溶媒１３及び電解液１
１は、このセトラ室１６ｃで静置され、水に不混和で水
より比重の小さい有機溶媒１３は上方に移動し電解液１
１は下方に移動して互いに分離される。このセトラ室１
６ｃで下方に移動することにより有機溶媒１３と分離し
た電解液１１はその後第１配管１８を介して電解槽１２
に導びかれ再び再生される。一方、セトラ室１６ｃで上
方に移動することにより電解液１１と分離した未分解の
有機溶媒１３はその後連結管１７ａを介して溶媒槽１７
に流入し、ポンプ１７ｄにより溶媒管１７ｃを介してミ
キサ室１６ａに再び導入されて分解される。[0017] C 6 H 6 + 42H 2 O + 30Ag 2+ → 6CO 2 ↑ + 30H 3 0 + + 30Ag + ... (1) electrolytic solution 11 from the electrolytic cell 12, by an organic solvent 13 is supplied from the solvent tank 17, a mixer From the chamber 16a, the undecomposed organic solvent 13 and the electrolytic solution 11 overflowing over the partition 16b flow into the settle chamber 16c as shown by the dashed arrow in the figure. The organic solvent 13 and the electrolyte 1 flowing in this way
1, the organic solvent 13 which is immiscible with water and has a lower specific gravity than water moves upward,
1 move downward and become separated from each other. This Setra Room 1
The electrolytic solution 11 separated from the organic solvent 13 by moving downward at 6 c is then supplied to the electrolytic cell 12 via the first pipe 18.
Guided to play again. On the other hand, the undecomposed organic solvent 13 separated from the electrolytic solution 11 by moving upward in the settling chamber 16c is then supplied to the solvent tank 17 via the connecting pipe 17a.
And is again introduced into the mixer chamber 16a via the solvent pipe 17c by the pump 17d to be decomposed.
【００１８】[0018]
【発明の効果】以上述べたように、本発明によれば、レ
ドックス種を酸化種として機能させる電解槽と、電解液
と有機溶媒とを撹拌手段により混合して有機溶媒を酸化
分解する反応槽とを備えたので、撹拌手段の混合により
有機溶媒と電解液の界面面積を増大することができる。
また、撹拌手段の撹拌により反応槽で使用した電解液を
電解槽に導きかつ電解槽の電解液を反応槽に導くように
構成したので、撹拌手段の撹拌により電解槽で生成した
酸化種を反応槽で直ちに有機溶媒の分解処理に寄与さ
せ、酸化種の有機溶媒との接触時間を確保して有機溶媒
の分解速度を十分に速めることができるとともに、電解
液を循環させるための特別の装置を不要にして装置自体
を簡素化することができる。As described above, according to the present invention, an electrolytic cell in which a redox species functions as an oxidizing species, and a reaction tank in which an electrolytic solution and an organic solvent are mixed by stirring means to oxidatively decompose the organic solvent. Therefore, the interface area between the organic solvent and the electrolytic solution can be increased by mixing the stirring means.
In addition, since the electrolytic solution used in the reaction tank is led to the electrolytic tank by the stirring means and the electrolytic solution in the electrolytic tank is led to the reaction tank, oxidizing species generated in the electrolytic tank by the stirring of the stirring means are reacted. A special device for circulating the electrolytic solution, while contributing to the decomposition treatment of the organic solvent immediately in the tank, ensuring the contact time of the oxidizing species with the organic solvent and sufficiently increasing the decomposition rate of the organic solvent, can be achieved. The device itself can be simplified by making it unnecessary.
【００１９】また、溶媒槽とこの溶媒槽に貯えられた有
機溶媒をミキサ室に導くポンプとを更に備えれば、この
溶媒槽をセトラ室における未分解の有機溶媒が流入可能
に構成することにより反応槽における有機溶媒と電解液
からなる液面を常に一定に保つことができる。更に、本
発明では、有機溶媒が常に循環するので、いわゆるバッ
チ処理及び連続処理の双方において使用することがで
き、従来必要とされた処理時間を考慮して被処理物を投
入する手間を省くことができる。また、比較的多くの被
処理物を投入した場合にあっても有機溶媒が反応槽から
溢れることはなく、多量の有機溶媒の連続処理が可能に
なる。Further, if the apparatus further comprises a solvent tank and a pump for guiding the organic solvent stored in the solvent tank to the mixer chamber, the solvent tank is configured to allow the undecomposed organic solvent in the settle chamber to flow therein. The liquid surface composed of the organic solvent and the electrolytic solution in the reaction tank can be always kept constant. Further, in the present invention, since the organic solvent is constantly circulated, the organic solvent can be used in both so-called batch processing and continuous processing, and it is possible to save the time and effort required to input an object to be treated in consideration of the conventionally required processing time. Can be. Further, even when a relatively large number of objects to be treated are charged, the organic solvent does not overflow from the reaction tank, and a large amount of the organic solvent can be continuously treated.
【図１】本発明の酸化分解装置の構成を示す概念図。FIG. 1 is a conceptual diagram showing a configuration of an oxidative decomposition device of the present invention.
１１ 水性電解液 １２ 電解槽 １２ａ 陽極 １２ｂ 陰極 １３ 有機溶媒 １４ 撹拌手段 １４ａ 電動モータ １４ｂ 回転軸 １４ｃ 回転翼 １６ 反応槽 １６ａ ミキサ室 １６ｂ 隔壁 １６ｃ セトラ室 １７ 溶媒槽 １７ｄ ポンプ １８ 第１配管 １９ 第２配管 DESCRIPTION OF SYMBOLS 11 Aqueous electrolytic solution 12 Electrolytic tank 12a Anode 12b Cathode 13 Organic solvent 14 Stirring means 14a Electric motor 14b Rotary shaft 14c Rotor blade 16 Reaction tank 16a Mixer room 16b Partition wall 16c Settler room 17 Solvent tank 17d Pump 18 1st piping 19 2nd piping
───────────────────────────────────────────────────── フロントページの続き (72)発明者 近沢 孝弘 茨城県那珂郡那珂町大字向山字六人頭1002 番地の14 三菱マテリアル株式会社環境・ エネルギー研究所内 Ｆターム(参考） 4K021 AB25 BA04 BA06 BA17 BC03 CA09 CA10 DB05 DB40 DB47 DC11 DC15 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Takahiro Chikazawa 1002, 6-head, Mukaiyama, Naka-cho, Naka-gun, Naka-gun, Ibaraki Prefecture F-term in Mitsubishi Materials Corporation Environment and Energy Research Laboratory (reference) CA09 CA10 DB05 DB40 DB47 DC11 DC15
Claims (4)
強力な酸化種として機能するレドックス種を含む水性電
解液(11)を貯え前記電解液中に配置された陽極(12a)と
陰極(12b)との間に電位差を与えることにより前記レド
ックス種を酸化種として機能させる電解槽(12)と、 前記酸化種を含む電解液(11)と水に不混和で水より比重
の小さい有機溶媒(13)とを撹拌手段(14)により混合して
前記有機溶媒(13)を酸化分解するミキサ室(16a)と、前
記ミキサ室(16a)に隔壁(16b)を隔てて隣接され前記隔壁
(16b)を越えて溢れた未分解の有機溶媒(13)及び前記電
解液(11)を静置することにより互いに分離するセトラ室
(16c)とを有する反応槽(16)とを備え、 前記撹拌手段(14)の撹拌により前記反応槽(16)で使用し
た電解液(11)を前記電解槽(12)に導きかつ前記電解槽(1
2)の電解液(11)を前記反応槽(16)に導くように構成され
た有機溶媒の酸化分解装置。1. An anode (12a) and a cathode (12b) containing an aqueous electrolyte solution (11) containing oxo acid as a main component and containing a redox species functioning as a strong oxidizing species by electrolytic oxidation, and arranged in the electrolyte solution. An electrolytic cell (12) that causes the redox species to function as an oxidizing species by giving a potential difference between the organic solvent (13) and an electrolyte (11) containing the oxidizing species and an organic solvent immiscible with water and having a lower specific gravity than water. And a mixing chamber (16a) for mixing and oxidatively decomposing the organic solvent (13) by stirring means (14), and the partition adjacent to the mixer chamber (16a) via a partition (16b).
(16b) The unsettled organic solvent (13) overflowing beyond (16b) and the electrolytic solution (11) are separated from each other by leaving the electrolyte solution (11) to stand.
(16c), and the electrolytic solution (11) used in the reaction tank (16) is guided to the electrolytic tank (12) by the stirring of the stirring means (14), and the electrolysis is performed. Tank (1
An organic solvent oxidative decomposition device configured to guide the electrolytic solution (11) of (2) to the reaction tank (16).
セトラ室(16c)で分離された未分解の有機溶媒(13)が流
入可能に構成された溶媒槽(17)と、前記溶媒槽(17)に貯
えられた有機溶媒(13)をミキサ室に導くポンプ(17d)と
を更に備えた請求項１記載の有機溶媒の酸化分解装置。2. A solvent tank (17) configured to store an organic solvent (13) to be oxidatively decomposed and to allow an undecomposed organic solvent (13) separated in a settling chamber (16c) to flow therein; The organic solvent oxidative decomposition apparatus according to claim 1, further comprising a pump (17d) for guiding the organic solvent (13) stored in the tank (17) to the mixer chamber.
設けられた電動モータ(14a)と、前記ミキサ室(16a)内に
鉛直に設けられ下端が前記ミキサ室(16a)の下部に達し
上端が前記電動モータ(14a)の回転軸に連結された回転
軸(14b)と、前記回転軸(14b)の下端に設けられ前記回転
軸(14b)とともに回転して電解液(11)及び有機溶媒(13)
を混合可能に構成された回転翼(14c)とを有し、 セトラ室(16c)の下部と電解槽(12)が第１配管(18)によ
り連結され、前記電解槽(12)と前記回転翼(14c)に臨む
ミキサ室(16a)の下部とが第２配管(19)により連結さ
れ、 前記回転翼(14c)の回転により前記第２配管(19)を介し
て前記電解槽(12)の電解液(11)を前記ミキサ室(16a)に
導きかつ前記第１配管(18)を介して前記セトラ室(16c)
の電解液(11)を前記電解槽(12)に導くように構成された
請求項１又は２記載の有機溶媒の酸化分解装置。3. A stirring means (14) is provided between the electric motor (14a) provided above the mixer chamber (16a) and the mixer chamber (16a). A rotating shaft (14b) reaching the lower end and having an upper end connected to the rotating shaft of the electric motor (14a); and a rotating shaft (14b) provided at the lower end of the rotating shaft (14b) to rotate together with the rotating shaft (14b) so that the electrolytic solution (11 ) And organic solvent (13)
And a rotating blade (14c) configured to be able to mix the lower part of the settling chamber (16c) and the electrolytic cell (12) by a first pipe (18). The lower part of the mixer chamber (16a) facing the blade (14c) is connected by a second pipe (19), and the electrolytic cell (12) is connected via the second pipe (19) by the rotation of the rotary blade (14c). To the mixer chamber (16a) and through the first pipe (18) to the settle chamber (16c).
The oxidative decomposition device for an organic solvent according to claim 1 or 2, wherein the electrolytic solution (11) is introduced into the electrolytic cell (12).
酸化によって強力な酸化種として機能するレドックス種
を含む水性電解液(11)を電解して前記レドックス種を酸
化種として機能させる工程と、 ミキサ室(16a)に水に不混和で水より比重の小さい有機
溶媒(13)を導入する工程と、 前記電解槽(12)の酸化種を含む電解液(11)をミキサ室(1
6a)に導入して有機溶媒(13)と混合することにより前記
有機溶媒(13)を酸化分解する工程と、 前記ミキサ室(16a)で未分解の有機溶媒(13)と前記電解
液(11)をセトラ室(16c)で静置して互いに分離する工程
と、 前記セトラ室(16c)で分離した電解液(11)を前記電解槽
(12)に戻す工程と、 前記セトラ室(16c)で分離した未分解の有機溶媒(13)を
再び前記ミキサ室(16a)に導入する工程とを含む有機溶
媒の酸化分解方法。4. An electrolytic cell (12) electrolyzes an aqueous electrolytic solution (11) containing oxoacid as a main component and a redox species which functions as a strong oxidizing species by electrolytic oxidation, so that the redox species functions as an oxidizing species. A step of introducing an organic solvent (13) that is immiscible with water and has a lower specific gravity than water into the mixer chamber (16a), and converts the electrolytic solution (11) containing the oxidizing species of the electrolytic cell (12) into the mixer chamber (16a). 1
Oxidatively decomposing the organic solvent (13) by being introduced into 6a) and mixing with the organic solvent (13), and the undecomposed organic solvent (13) and the electrolytic solution (11) in the mixer chamber (16a). ) In a settling chamber (16c) to separate them from each other, and the electrolytic solution (11) separated in the settling chamber (16c)
A method for oxidatively decomposing an organic solvent, comprising a step of returning to (12) and a step of introducing again the undecomposed organic solvent (13) separated in the settle chamber (16c) into the mixer chamber (16a).
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP11169440A JP2000355784A (en) | 1999-06-16 | 1999-06-16 | Oxidation decomposition apparatus of organic solvent and oxidation decomposition method therefor |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP11169440A JP2000355784A (en) | 1999-06-16 | 1999-06-16 | Oxidation decomposition apparatus of organic solvent and oxidation decomposition method therefor |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JP2000355784A true JP2000355784A (en) | 2000-12-26 |
Family
ID=15886654
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP11169440A Withdrawn JP2000355784A (en) | 1999-06-16 | 1999-06-16 | Oxidation decomposition apparatus of organic solvent and oxidation decomposition method therefor |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2000355784A (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2005528627A (en) * | 2002-06-01 | 2005-09-22 | バイオダイナミックス リサーチ リミテッド | New collection process |
| CN103451683A (en) * | 2012-05-28 | 2013-12-18 | 中国原子能科学研究院 | On-line electrolytic mixing clarifying tank |
-
1999
- 1999-06-16 JP JP11169440A patent/JP2000355784A/en not_active Withdrawn
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2005528627A (en) * | 2002-06-01 | 2005-09-22 | バイオダイナミックス リサーチ リミテッド | New collection process |
| US7807040B2 (en) | 2002-06-01 | 2010-10-05 | Biodynamics Research Limited | Recovery process |
| CN103451683A (en) * | 2012-05-28 | 2013-12-18 | 中国原子能科学研究院 | On-line electrolytic mixing clarifying tank |
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