EP2257949B1 - Procédé pour le conditionnement d'une solution de nettoyage résultant du nettoyage par voie humide d'un générateur de vapeur nucléaire - Google Patents

Procédé pour le conditionnement d'une solution de nettoyage résultant du nettoyage par voie humide d'un générateur de vapeur nucléaire Download PDF

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Publication number
EP2257949B1
EP2257949B1 EP09725983.2A EP09725983A EP2257949B1 EP 2257949 B1 EP2257949 B1 EP 2257949B1 EP 09725983 A EP09725983 A EP 09725983A EP 2257949 B1 EP2257949 B1 EP 2257949B1
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EP
European Patent Office
Prior art keywords
cleaning solution
cleaning
cathode
conditioning
steam generator
Prior art date
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Active
Application number
EP09725983.2A
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German (de)
English (en)
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EP2257949A1 (fr
Inventor
Rainer Gassen
Christian Topf
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.)
Areva GmbH
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Areva GmbH
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Publication of EP2257949A1 publication Critical patent/EP2257949A1/fr
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04—Treating liquids
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • G21F9/16—Processing by fixation in stable solid media

Definitions

  • the invention relates to a method for conditioning a resulting in the wet-chemical cleaning of a nuclear steam generator cleaning solution.
  • the resulting cleaning solutions When wet-cleaning a nuclear steam generator, the resulting cleaning solutions must be disposed of. These are usually in dissolved form complexing agent, ammonium, amines and iron. The used cleaning solutions are burnt in many cases as hazardous waste. However, special disposal problems arise when the cleaning solutions contain radioactive metallic nuclides, for example Co60, in concentrations above an allowable limit. These spent cleaning solutions can therefore not be treated as normal waste, but must be conditioned for final disposal very complex and expensive and spent in special repository.
  • radioactive metallic nuclides for example Co60
  • the invention is therefore based on the object, a method for conditioning a resulting in the wet-chemical cleaning of a nuclear steam generator cleaning solution with which also the disposal of cleaning solutions contaminated with radioactive metal nuclides is economically possible.
  • the above object is achieved according to the invention by a method having the features of claim 1. Since the cleaning solution is treated electrolytically and radioactive metal nuclides contained in the cleaning solution are deposited on a cathode, it is possible to reduce the radioactive contamination of the cleaning solution so far that it is below a predetermined exemption limit. In this way, the disposal of the present in a large amount cleaning solution is considerably simplified, since only the radioactively contaminated cathode must be disposed of as radioactive waste in compliance with the respective radiation protection and disposal conditions.
  • the cathode is a diamond electrode and therefore consists of a material which has a hydrogen overvoltage and whose potential is set above the potential of hydrogen evolution, a particularly effective deposition of radioactive metallic nuclides is achieved.
  • the anode also consists of a material which has an oxygen overvoltage, preferably also a diamond electrode whose potential is below the Potential of the oxygen evolution is adjusted, the organic components in the cleaning solution, such as a complexing agent, can be denatured during electrolysis at the same time, so that almost all Fe precipitates as oxide or hydroxide. Due to the large surface area of the precipitated iron oxide or iron hydroxide, radioactive metal nuclides, for example Co60, which are still present in the solution are also adsorbed thereon and thus removed from the cleaning solution in this way. If the electrolysis time is long enough, the entire complexing agent (eg EDTA) can be destroyed.
  • a complexing agent eg EDTA
  • the COD or TOC value (chemical oxygen demand or total content of organic carbon) drops significantly in this treatment. In this way it is possible to reduce the contamination with both organic compounds and with radioactive nuclides so far that the solution can be disposed of with little effort. Only precipitate and cathode have to be disposed of as radioactive waste with a considerably lower volume.
  • a disposal of the cathode is not required, that is, their further use is possible if the deposited on their metals with an inorganic acid are removed.
  • the neutralized acid has to be disposed of together with a precipitate (FeO, Fe 2 O 3 , Fe (OH) 2 , Fe (OH) 3 ) which may be formed by destroying the complexing agents.
  • a two-stage electrolysis is carried out, in which the cleaning solution is acidified after a first electrolytic treatment and subsequently subjected to a second electrolytic treatment becomes.
  • the cleaning solution is electrolyzed without pretreatment.
  • the dissolved Fe is deposited and additionally precipitated when using an anode with oxygen overvoltage.
  • the cleaning solution pre-treated in this way is acidified and re-electrolyzed until the concentration of activity (Co60) is below a predetermined release limit. After that it can be neutralized and disposed of.
  • a simulated DE cleaning solution (1.3 l) with 10 g / l EDTA, 11.8 g / l morpholine, corresponding to a COD of 29.2 g / l, 106 mg / l Co and 2.1 g / l Fe was electrolyzed on diamond electrodes (cathode and anode). After 6 h at 1.0 A / m 2 , the cleaning solution (in the diagram of Fig.1 graphically represented by bars I) only 0.3% of the Fe and 31% of the Co. On the cathode (in the diagram of Fig.1 represented by bars II), 1.5% of the Fe and 51% of the Co were deposited. 98.2% of the Fe and 18% of the Co were in precipitation (in the diagram of the Fig.1 illustrated by the bars III) adsorbed. The EDTA was 96% decomposed, the COD value reduced by about 50%.
  • the cleaning solution treated in this way was filtered, the filtrate acidified (pH ⁇ 2) and re-electrolyzed in a subsequent treatment step for 8 h at 2.0 A / m 2 .
  • the filtrate acidified (pH ⁇ 2) was re-electrolyzed in a subsequent treatment step for 8 h at 2.0 A / m 2 .
  • the filtrate acidified (pH ⁇ 2) was re-electrolyzed in a subsequent treatment step for 8 h at 2.0 A / m 2 .
  • 6.3 mg / l Fe 6.0 mg / l were on the cathode (in the diagram of the Fig.2 graphically represented by bars II), so that now 0.28% and only 0.4 mg / l or 0.02% of the solution originally dissolved in the cleaning solution (bar I) were present on the cathode.
  • the final values of the EDTA content and the COD value were reached at 0.01 g / l and 0.16 g / l, respectively. Both the content of EDTA and the COD value were reduced by more than 99% by the combined treatment.
  • a simulated cleaning solution (1.3 l) containing 10 g / l EDTA, 11.8 g / l morpholine, corresponding to a COD of 29.2 g / l, 63 mg / l Co, and 1.96 g / l Fe was acidified in a first step to a pH of about 2 and electrolyzed for 8h at 2000 A / m 2 .
  • 92% of the originally dissolved Co and 89% of the originally dissolved Fe were deposited on the cathode.
  • the COD content in the solution was only 0.29 g / L and the content of EDTA in the solution was reduced to 0.25 g / L.
  • the Fe and Co deposited on the cathode are removed with an acid, eg sulfuric acid, the solution is then neutralized and evaporated. Otherwise, Fe and Co can be removed anodically after acidification. The resulting solution can then be neutralized with NH 3 and then likewise evaporated.
  • an acid eg sulfuric acid
  • Example 2 The advantage of such an acidic single-stage electrolysis according to Example 2 consists essentially in the fact that the steps required in Example 1, filtration and re-electrolysis omitted.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Water Treatment By Electricity Or Magnetism (AREA)
  • Electrolytic Production Of Metals (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)

Claims (5)

  1. Procédé de conditionnement d'une solution de nettoyage produite lors du nettoyage chimique par voie humide d'un générateur de vapeur nucléaire, dans lequel la solution de nettoyage subit un traitement électrolytique et les nucléides métalliques radioactifs contenus dans la solution de nettoyage sont déposés sur une cathode, dans lequel la cathode est une électrode au diamant, dont le potentiel est réglé au-dessus du potentiel de développement d'hydrogène.
  2. Procédé selon la revendication 1, dans lequel les métaux déposés sur la cathode sont dissous avec un acide.
  3. Procédé selon les revendications 1 ou 2, dans lequel la solution de nettoyage est acidifiée après le traitement électrolytique et est ensuite soumise à un nouveau traitement électrolytique.
  4. Procédé selon une des revendications précédentes, dans lequel l'anode est constituée d'un matériau, qui présente une surtension d'oxygène, et dans lequel le potentiel de l'anode est réglé au-dessous du potentiel de développement d'oxygène.
  5. Procédé selon la revendication 4, dans lequel l'anode est une électrode au diamant.
EP09725983.2A 2008-03-28 2009-03-20 Procédé pour le conditionnement d'une solution de nettoyage résultant du nettoyage par voie humide d'un générateur de vapeur nucléaire Active EP2257949B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102008016020A DE102008016020A1 (de) 2008-03-28 2008-03-28 Verfahren zum Konditionieren einer bei der nasschemischen Reinigung eines nuklearen Dampferzeugers anfallenden Reinigungslösung
PCT/EP2009/053329 WO2009118277A1 (fr) 2008-03-28 2009-03-20 Procédé pour le conditionnement d'une solution de nettoyage résultant du nettoyage par voie humide d'un générateur de vapeur nucléaire

Publications (2)

Publication Number Publication Date
EP2257949A1 EP2257949A1 (fr) 2010-12-08
EP2257949B1 true EP2257949B1 (fr) 2013-05-08

Family

ID=40765778

Family Applications (1)

Application Number Title Priority Date Filing Date
EP09725983.2A Active EP2257949B1 (fr) 2008-03-28 2009-03-20 Procédé pour le conditionnement d'une solution de nettoyage résultant du nettoyage par voie humide d'un générateur de vapeur nucléaire

Country Status (8)

Country Link
US (1) US20100252449A1 (fr)
EP (1) EP2257949B1 (fr)
JP (1) JP5343121B2 (fr)
KR (1) KR20100077014A (fr)
DE (1) DE102008016020A1 (fr)
ES (1) ES2411932T3 (fr)
TW (1) TW200945369A (fr)
WO (1) WO2009118277A1 (fr)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112144066B (zh) * 2020-09-30 2022-03-25 西安热工研究院有限公司 高温气冷堆核电机组二回路水汽系统化学清洗剂及清洗方法

Family Cites Families (23)

* Cited by examiner, † Cited by third party
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JPS5851977A (ja) * 1981-09-25 1983-03-26 Hitachi Ltd 化学除染液の再生方法
JPS6093999A (ja) * 1983-10-28 1985-05-25 日立プラント建設株式会社 化学除染廃液の処理方法
JPH0631858B2 (ja) * 1984-09-26 1994-04-27 株式会社東芝 溶液中金属イオンの分離方法
JPS61194398A (ja) * 1985-02-23 1986-08-28 株式会社東芝 放射能で汚染された被処理物の除染装置
JPS61231496A (ja) * 1985-04-05 1986-10-15 日立プラント建設株式会社 放射性金属廃棄物の除染方法
JPS6336198A (ja) * 1986-07-29 1988-02-16 株式会社東芝 放射性廃液の処理方法
US4861444A (en) * 1988-09-06 1989-08-29 Schoessow Glen J Process for treating radioactive material to make it safe for disposal
JPH02171695A (ja) * 1988-12-26 1990-07-03 Toshiba Corp 放射性廃液処理装置
US5122268A (en) * 1989-08-11 1992-06-16 Westinghouse Electric Corp. Apparatus for waste disposal of radioactive hazardous waste
JPH0438499A (ja) * 1990-06-04 1992-02-07 Toshiba Corp 除染廃液の処理方法
JP2713828B2 (ja) * 1992-01-14 1998-02-16 動力炉・核燃料開発事業団 核燃料再処理溶解液から有価金属を回収する方法
FR2690270A1 (fr) * 1992-04-21 1993-10-22 Framatome Sa Enceinte de séparation et de confinement de produits radioactifs contenus dans des effluents liquides et installation et procédé pour le traitement de ces effluents.
JPH05341098A (ja) * 1992-06-11 1993-12-24 Mitsubishi Heavy Ind Ltd 蒸気発生器二次側化学洗浄液の処理方法
FR2717459B1 (fr) * 1994-03-16 1996-04-12 Commissariat Energie Atomique Procédé et installation de destruction de solutes organiques, en particulier d'agents complexants, présents dans une solution aqueuse telle qu'un effluent radioactif.
FR2736631B1 (fr) * 1995-07-11 1997-10-10 Framatome Sa Procede de traitement par electrolyse d'un effluent liquide contenant des metaux dissous et application au traitement d'effluents contenant du cerium
JPH10104396A (ja) * 1996-10-02 1998-04-24 Toshiba Corp 化学除染方法およびその装置
GB2319040B (en) * 1996-11-08 2000-07-12 Aea Technology Plc Radioactive effluent treatment
FR2761085B1 (fr) * 1997-03-24 1999-04-16 Commissariat Energie Atomique Procede electrolytique de recuperation et de recyclage de l'argent a partir d'une solution nitrique
DE19842396A1 (de) * 1998-09-16 2000-04-13 Fraunhofer Ges Forschung Elektrode für elektrochemische Prozesse
US6149797A (en) * 1998-10-27 2000-11-21 Eastman Kodak Company Method of metal recovery using electrochemical cell
DE10005681B4 (de) * 2000-02-07 2005-06-16 Atc Dr. Mann E.K. Verfahren und Vorrichtung zur Dekontamination metallhaltiger Wässer
US6682646B2 (en) * 2002-03-25 2004-01-27 Electric Power Research Institute Electrochemical process for decontamination of radioactive materials
JP2004321963A (ja) * 2003-04-25 2004-11-18 Kurita Water Ind Ltd 硝酸性窒素含有水の処理方法

Also Published As

Publication number Publication date
JP5343121B2 (ja) 2013-11-13
KR20100077014A (ko) 2010-07-06
WO2009118277A1 (fr) 2009-10-01
TW200945369A (en) 2009-11-01
EP2257949A1 (fr) 2010-12-08
ES2411932T3 (es) 2013-07-09
DE102008016020A1 (de) 2009-10-01
JP2011515687A (ja) 2011-05-19
US20100252449A1 (en) 2010-10-07

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