EP2188814A2 - Procédé de décontamination de surfaces d'installations nucléaires contaminées par des rayons alpha - Google Patents

Procédé de décontamination de surfaces d'installations nucléaires contaminées par des rayons alpha

Info

Publication number
EP2188814A2
EP2188814A2 EP08786183A EP08786183A EP2188814A2 EP 2188814 A2 EP2188814 A2 EP 2188814A2 EP 08786183 A EP08786183 A EP 08786183A EP 08786183 A EP08786183 A EP 08786183A EP 2188814 A2 EP2188814 A2 EP 2188814A2
Authority
EP
European Patent Office
Prior art keywords
ppm
oxide
oxalic acid
surfactant
carried out
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.)
Granted
Application number
EP08786183A
Other languages
German (de)
English (en)
Other versions
EP2188814B1 (fr
Inventor
Rainer Gassen
Christoph Stiepani
Horst-Otto Bertholdt
Bertram Zeiler
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
Original Assignee
Areva NP GmbH
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Areva NP GmbH filed Critical Areva NP GmbH
Publication of EP2188814A2 publication Critical patent/EP2188814A2/fr
Application granted granted Critical
Publication of EP2188814B1 publication Critical patent/EP2188814B1/fr
Not-in-force legal-status Critical Current
Anticipated expiration legal-status Critical

Links

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
    • G21F9/001—Decontamination of contaminated objects, apparatus, clothes, food; Preventing contamination thereof
    • G21F9/002—Decontamination of the surface of objects with chemical or electrochemical processes
    • G21F9/004—Decontamination of the surface of objects with chemical or electrochemical processes of metallic surfaces
    • 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
    • G21F9/12—Processing by absorption; by adsorption; by ion-exchange
    • 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
    • G21F9/28—Treating solids

Definitions

  • the invention relates to methods for the decontamination of surface contaminated with alpha emitters of nuclear facilities, such as decontamination of the surface of components of the coolant system of nuclear power plants, to which reference is made below by way of example.
  • radioactive oxide layers are formed on the internal surfaces of components of the coolant system, such as pipes, pumps, steam generator pipes, which must be removed in the event of the decommissioning of a decommissioned nuclear power plant in order to reduce the radioactive radiation of the components to tolerable levels.
  • the removal of the oxide layer on component surfaces is effected, for example, by a two-stage decontamination process in which the oxide layer is pretreated in the first stage with a strong oxidizing agent such as potassium permanganate or permanganic acid and in a second step the oxide layer is dissolved with a cleaning solution containing one or more complexing acids.
  • the spent cleaning solution containing the constituents of the oxide layer in dissolved form is either evaporated to a residual amount or passed through ion exchangers to remove the ionic form of the oxide layer from the cleaning solution. Exhausted ion exchange material and the residual amount of tion solution are fed in an appropriate form an intermediate or final storage.
  • EP 753196 Bl discloses a method for disposal of an aqueous cleaning solution previously used to remove ferritic deposits.
  • the cleaning solution comprises an organic acid as well as ferritic deposits dissolved in the form of iron complexes.
  • the disclosed process makes it possible to convert the entire organic acid into CO2 and water by means of a cyclic process. After carrying out this cyclic process, only a relatively small amount of iron salt remains in the solution, which can be removed with the aid of a cation exchanger. Since the cyclic process presupposes the presence of iron ions in the cleaning solution, they are initially supplied to the cleaning solution, provided that they are not already present in sufficient concentration as a result of the preceding decontamination.
  • gamma adhesives such as Cr-51 and Co-60 are detected.
  • These nuclides are to a large extent present, for example, incorporated in an oxide layer of a component, in the form of their oxides, these being from the active substances of conventional decontamination solutions.
  • complexing acids are relatively easily dissolved.
  • transuranic elements like Am-241 are partially solved.
  • oxide particles which are not visible to the naked eye and which contain alpha emitters or are bound to the alpha emitters remain. These particles only adhere loosely to the surface of the components previously freed of their oxide layer, so that the alpha emitters can be partially wiped off with a cloth, for example during a wipe test.
  • gamma-emitting particles may also be present on a component surface.
  • the components of the coolant system are to be recycled, which is only possible if the radioactivity measured on a component is lower than the specified limit values with regard to gamma and beta radiation as well as alpha radiation.
  • US 2003/0172959 A1 discloses a process for surface decontamination.
  • the cleaning solution proposed for this purpose contains a surfactant as wetting agent and a ketoamine as active cleaning component.
  • the cleaning solution may additionally be provided with an acid, for example oxalic acid.
  • the used cleaning solution is drained and collected in a suitable container.
  • the spent cleaning solution is now an unspecified, commonplace Disposal procedures, such as evaporation available.
  • the surfaces of the components are treated according to claim 1 with an aqueous solution containing oxalic acid in addition to a cationic and / or zwitterionic surfactant.
  • Such treatment will be carried out following a decontamination procedure, with the exception of the
  • the particles may consist of the oxide of an alpha emitter. It can also be other particles adhere to the surface of alpha emitters.
  • the proportion of alpha-emitting nuclides (in the following abbreviated to alphanuclides) can be lowered so far that the surfaces have an activity of less than 0.1 Bq / cm 2 .
  • the ratio of gamma to alpha decay results in values that often exceed a threshold of 10 significantly. If this limit value is detected for the components, their release, for example for recycling, requires only measurements of the gamma radiation, which is possible with simple devices and in a short time. If a limit of 10 can not be established, time-consuming and complex measurements of the alpha radiation must be carried out and the personnel must be monitored in a time- and cost-intensive manner by means of elimination analyzes for the incorporation of alphanuclides.
  • the particles in question adhering to a component surface pass into the solution, but also Gamoma activity present on the surface is reduced.
  • the aqueous solution is passed through a cation exchanger before it is optimally subjected to a further treatment, for example by evaporation, or reused.
  • a further treatment for example by evaporation, or reused.
  • the bound to the surfactants alpha activity passes to the ion exchanger.
  • the oxalic acid remains in the solution and can be removed, for example, by the method disclosed in EP 0 753 196.
  • the method according to the invention is carried out following a generally known decontamination method aimed at the removal of oxide layers, wherein it is particularly advantageous if oxalic acid is already used in this method.
  • the addition of oxalic acid is then unnecessary or at least only to a lesser extent required.
  • To remove the particles dissolved out of the oxide layers mainly metal ions, at least part of the solution is passed over an ion exchanger, preferably via a cation exchanger.
  • the appropriate oxalic acid concentration depends i.a. However, depending on the nature and thickness of the oxide layers to be removed, it should in any case be at least 250 ppm.
  • the upper limit of the oxalic acid concentration is 15,000 ppm. Other levels are barely associated with a significant effect.
  • a surfactant which is particularly suitable for carrying out the process according to the invention must, on the one hand, be effective in cooperation with oxalic acid with regard to the detachment of particles from surfaces. On the other hand, it must mediate the binding of the particles to a cation exchanger, so that they can be removed from the solution at least in part.
  • amino acids of the general formula HOOC-R-NH 2 having an aliphatic radical of 4 to 24 carbon atoms and N-oxides of the general formula R 1 - (NO) (R 2 ) (R 3) have been found, in the latter Case as aliphatic radicals Rl having 4 to 24 carbon atoms and R2 and R3 are each having 1 to 10 carbon atoms. Particular preference is given here to N-oxides in which R 1 comprises 12 to 24 C atoms and R 2 and R 3 comprise 1 to 3 C atoms.
  • dimethyl-octadecylamine-N-oxide has emerged as the best-acting surfactant.
  • a treatment at elevated temperature of more than 30 0 C is appropriate.
  • a temperature of at least 50 ° C. is preferred, the upper limit being 200 ° C.
  • concentration of the particular surfactant used depends i.a. its chemical structure and the resulting effectiveness, as well as the type and thickness of the oxide coatings.
  • a concentration range covering a wide range of applications is between 50 ppm and 3000 ppm.
  • the samples were placed in a container with an aqueous solution containing a surfactant at a concentration of at least 150 ppm, 350 ppm and 2000 ppm, respectively, and oxalic acid in a concentration above 50 ppm.
  • the samples were treated for between 5 and 40 hours at an elevated temperature of 50 ° C. to 200 ° C.
  • Americium-241 alpha-brier
  • cobalt-60 gamma-emitter
  • Americium was chosen because it can be determined by relatively simple means via gamma radiation accompanying its alpha decay.
  • measurements were carried out in the untreated state (there is an oxide layer formed in power plant operation), after the oxide layer has been removed and after treatment with a solution containing a surfactant and oxalic acid, and the respective ratio of the gamma activity to the alpha activity calculated.
  • a ratio of gamma to alpha activity (Co-60 / Am-241) is often found to be smaller than the corresponding ratio for the as yet untreated components or their surfaces, ie the relative proportion of alpha emitters has increased.
  • the method according to the invention is used-in the case of the tests in question, it was carried out after conventional oxide detachment-a large proportion of the alphanuclides present on the component surface are removed, which is reflected in the gamma / alpha ratio. This increased by a factor of about 500 in test 1, by a factor of about 6 in test 2 and by a factor of about 10 in test 3.
  • the conventional treatment ends in metallically bright surfaces, but often have intolerable residual activity which could not be further reduced by known chemical processes.
  • the residual activities or the decontamination factors (DF) can be drastically reduced by 6 to 90 times for Co-60 and 20 to 350 times for Am-241 ,
  • the remaining solution can be further treated by destroying the oxalic acid present in it under the action of UV radiation and then for further purification over a Solid bed is passed.
  • the solution can then be reused or evaporated for disposal.

Landscapes

  • Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • General Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Food Science & Technology (AREA)
  • Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Detergent Compositions (AREA)
  • Cleaning By Liquid Or Steam (AREA)
  • Agricultural Chemicals And Associated Chemicals (AREA)

Abstract

L'invention concerne un procédé de décontamination de surfaces d'installations nucléaires contaminées par des rayons alpha, procédé mis en oeuvre comme complément à un procédé de décontamination ayant pour but d'éliminer les couches d'oxydes. Le procédé est caractérisé en ce que les surfaces sont traitées par une solution aqueuse renfermant un agent tensio-actif cationique ou ionique dipolaire et de l'acide oxalique, et en ce qu'au moins une partie de la solution est envoyée, après avoir agi sur une surface, sur un échangeur d'ions.
EP08786183A 2007-08-17 2008-07-16 Procédé de décontamination de surfaces d'installations nucléaires contaminées par des rayons alpha Not-in-force EP2188814B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102007038947A DE102007038947A1 (de) 2007-08-17 2007-08-17 Verfahren zur Dekontamination von mit Alphastrahlern kontaminierten Oberflächen von Nuklearanlagen
PCT/EP2008/059289 WO2009024417A2 (fr) 2007-08-17 2008-07-16 Procédé de décontamination de surfaces d'installations nucléaires contaminées par des rayons alpha

Publications (2)

Publication Number Publication Date
EP2188814A2 true EP2188814A2 (fr) 2010-05-26
EP2188814B1 EP2188814B1 (fr) 2012-09-12

Family

ID=40279852

Family Applications (1)

Application Number Title Priority Date Filing Date
EP08786183A Not-in-force EP2188814B1 (fr) 2007-08-17 2008-07-16 Procédé de décontamination de surfaces d'installations nucléaires contaminées par des rayons alpha

Country Status (9)

Country Link
US (1) US8702868B2 (fr)
EP (1) EP2188814B1 (fr)
JP (1) JP5235216B2 (fr)
KR (1) KR101182925B1 (fr)
CN (1) CN101809675B (fr)
CA (1) CA2695691C (fr)
DE (1) DE102007038947A1 (fr)
ES (1) ES2393291T3 (fr)
WO (1) WO2009024417A2 (fr)

Families Citing this family (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102009002681A1 (de) * 2009-02-18 2010-09-09 Areva Np Gmbh Verfahren zur Dekontamination radioaktiv kontaminierter Oberflächen
JP6009218B2 (ja) * 2011-05-24 2016-10-19 ローム アンド ハース エレクトロニック マテリアルズ エルエルシーＲｏｈｍ ａｎｄ Ｈａａｓ Ｅｌｅｃｔｒｏｎｉｃ Ｍａｔｅｒｉａｌｓ ＬＬＣ アルファ粒子放射体除去
EP3033751B1 (fr) * 2013-08-14 2019-10-23 Framatome GmbH Procédé pour la réduction de la contamination radioactive d'une surface d'une composante utilisée dans un reacteur nucléair
CN104900285B (zh) * 2015-04-08 2017-11-07 武汉网绿环境技术咨询有限公司 一种含放射性核素污染物的治理方法
KR200490490Y1 (ko) 2018-09-11 2019-11-19 채원영 샤워식 방사능 제염시스템

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CH653466A5 (de) * 1981-09-01 1985-12-31 Industrieorientierte Forsch Verfahren zur dekontamination von stahloberflaechen und entsorgung der radioaktiven stoffe.
DE3413868A1 (de) 1984-04-12 1985-10-17 Kraftwerk Union AG, 4330 Mülheim Verfahren zur chemischen dekontamination von metallischen bauteilen von kernreaktoranlagen
US4729855A (en) * 1985-11-29 1988-03-08 Westinghouse Electric Corp. Method of decontaminating radioactive metal surfaces
US4752206A (en) * 1987-04-06 1988-06-21 Johnson Service Company Take-out assembly for blow molding machine
CA2049728A1 (fr) * 1990-08-24 1992-02-25 Kenji Kitamura Composition de lavage capable de prevenir et d'ameliorer les irritations de la peau
US5278743A (en) * 1992-11-20 1994-01-11 Westinghouse Electric Corp. Alkaline-permanganate process
US5958247A (en) * 1994-03-28 1999-09-28 Siemens Aktiengesellschaft Method for disposing of a solution containing an organic acid
DE4410747A1 (de) 1994-03-28 1995-10-05 Siemens Ag Verfahren und Einrichtung zum Entsorgen einer Lösung, die eine organische Säure enthält
US6028113A (en) * 1995-09-27 2000-02-22 Sunburst Chemicals, Inc. Solid sanitizers and cleaner disinfectants
JPH09159798A (ja) * 1995-12-12 1997-06-20 Jgc Corp 泡除染および除染廃液処理の方法
US5752206A (en) * 1996-04-04 1998-05-12 Frink; Neal A. In-situ decontamination and recovery of metal from process equipment
WO2002004707A1 (fr) * 2000-07-11 2002-01-17 Ebara Industrial Cleaning Co., Ltd Agent de traitement de surface pour element metallique
US6652661B2 (en) * 2001-10-12 2003-11-25 Bobolink, Inc. Radioactive decontamination and translocation method
FR2841802B1 (fr) * 2002-07-08 2005-03-04 Commissariat Energie Atomique Composition, mousse et procede de decontamination de surfaces
JP2007198736A (ja) * 2006-01-23 2007-08-09 Mitsui Eng & Shipbuild Co Ltd 有機物含有放射性固体廃棄物の処理方法

Non-Patent Citations (1)

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See references of WO2009024417A3 *

Also Published As

Publication number Publication date
DE102007038947A1 (de) 2009-02-26
CA2695691A1 (fr) 2009-02-26
CN101809675A (zh) 2010-08-18
EP2188814B1 (fr) 2012-09-12
ES2393291T3 (es) 2012-12-20
CA2695691C (fr) 2014-10-21
KR20100057040A (ko) 2010-05-28
CN101809675B (zh) 2013-08-21
JP2010537160A (ja) 2010-12-02
WO2009024417A2 (fr) 2009-02-26
US8702868B2 (en) 2014-04-22
JP5235216B2 (ja) 2013-07-10
WO2009024417A3 (fr) 2009-04-23
KR101182925B1 (ko) 2012-09-13
US20100116288A1 (en) 2010-05-13

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