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 PDFInfo
- 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
- Authority
- EP
- European Patent Office
- Prior art keywords
- cleaning solution
- cleaning
- cathode
- conditioning
- steam generator
- 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.)
- Active
Links
- 238000004140 cleaning Methods 0.000 title claims description 34
- 238000000034 method Methods 0.000 title claims description 10
- 239000000126 substance Substances 0.000 title claims description 5
- 230000003750 conditioning effect Effects 0.000 title claims description 4
- 230000002285 radioactive effect Effects 0.000 claims description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 6
- 229910052760 oxygen Inorganic materials 0.000 claims description 6
- 239000001301 oxygen Substances 0.000 claims description 6
- 229910003460 diamond Inorganic materials 0.000 claims description 5
- 239000010432 diamond Substances 0.000 claims description 5
- 239000002184 metal Substances 0.000 claims description 5
- 229910052751 metal Inorganic materials 0.000 claims description 5
- 239000002253 acid Substances 0.000 claims description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 3
- 229910052739 hydrogen Inorganic materials 0.000 claims description 3
- 239000001257 hydrogen Substances 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 3
- 150000002739 metals Chemical class 0.000 claims description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 20
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 description 7
- 238000005868 electrolysis reaction Methods 0.000 description 7
- 238000010586 diagram Methods 0.000 description 5
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 4
- YNAVUWVOSKDBBP-UHFFFAOYSA-N Morpholine Chemical compound C1COCCN1 YNAVUWVOSKDBBP-UHFFFAOYSA-N 0.000 description 4
- 239000008139 complexing agent Substances 0.000 description 4
- 229910052742 iron Inorganic materials 0.000 description 4
- 239000002244 precipitate Substances 0.000 description 4
- 238000011109 contamination Methods 0.000 description 3
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- 239000002901 radioactive waste Substances 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- 230000001143 conditioned effect Effects 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000000706 filtrate Substances 0.000 description 1
- 239000002920 hazardous waste Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 239000004615 ingredient Substances 0.000 description 1
- 239000003456 ion exchange resin Substances 0.000 description 1
- 229920003303 ion-exchange polymer Polymers 0.000 description 1
- 235000014413 iron hydroxide Nutrition 0.000 description 1
- NCNCGGDMXMBVIA-UHFFFAOYSA-L iron(ii) hydroxide Chemical compound [OH-].[OH-].[Fe+2] NCNCGGDMXMBVIA-UHFFFAOYSA-L 0.000 description 1
- 150000007522 mineralic acids Chemical class 0.000 description 1
- 238000006386 neutralization reaction Methods 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 230000020477 pH reduction Effects 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
Images
Classifications
-
- 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.
Landscapes
- 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)
- 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.
- Procédé selon la revendication 1, dans lequel les métaux déposés sur la cathode sont dissous avec un acide.
- 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.
- 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.
- Procédé selon la revendication 4, dans lequel l'anode est une électrode au diamant.
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)
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)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
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 |
-
2008
- 2008-03-28 DE DE102008016020A patent/DE102008016020A1/de not_active Withdrawn
-
2009
- 2009-03-20 EP EP09725983.2A patent/EP2257949B1/fr active Active
- 2009-03-20 JP JP2011501182A patent/JP5343121B2/ja active Active
- 2009-03-20 KR KR1020107010170A patent/KR20100077014A/ko not_active Application Discontinuation
- 2009-03-20 WO PCT/EP2009/053329 patent/WO2009118277A1/fr active Application Filing
- 2009-03-20 ES ES09725983T patent/ES2411932T3/es active Active
- 2009-03-26 TW TW098109823A patent/TW200945369A/zh unknown
-
2010
- 2010-06-17 US US12/817,366 patent/US20100252449A1/en not_active Abandoned
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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