EP2188814B1 - 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 Download PDFInfo
- Publication number
- EP2188814B1 EP2188814B1 EP08786183A EP08786183A EP2188814B1 EP 2188814 B1 EP2188814 B1 EP 2188814B1 EP 08786183 A EP08786183 A EP 08786183A EP 08786183 A EP08786183 A EP 08786183A EP 2188814 B1 EP2188814 B1 EP 2188814B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- ppm
- atoms
- oxide
- oxalic acid
- surfactant
- 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.)
- Not-in-force
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 residual amount of cleaning solution remaining on evaporation be fed in an appropriate form an intermediate or final storage.
- EP 753 196 B1 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 CO 2 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 supplied to the cleaning solution at the beginning, as far as they are not already present in sufficient concentration by the previous decontamination.
- nuclides such as Cr-51 and Co-60 are detected.
- These nuclides are to a large extent, 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, for example relatively easily dissolved by complexing acids.
- 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 should be recycled, which is only possible if the radioactivity measured on a component is below the specified limit values with regard to gamma and beta radiation as well as alpha radiation.
- US 2003/0172959 A1 discloses a method 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 object of the invention to propose a method with which can be easily and effectively removed on surfaces of nuclear facilities, for example components of the coolant system of nuclear power alpha emitters, in particular, the radioactive residual waste should be kept as low as possible.
- 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 is carried out following a decontamination process which has at least partially removed oxide layers present on the surfaces.
- At least part of the aqueous solution is passed through an ion exchanger after being exposed to a surface.
- 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 with little time expenditure. 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 precipitation analyzes for the incorporation of alphanuclides.
- the particles in question adhering to a component surface pass into the solution, but also gamma 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, for example, with the EP 0 753 196 Procedures are removed.
- the process according to the invention is carried out following a generally known decontamination process aimed at the removal of oxide layers, wherein it is particularly advantageous if oxalic acid is already used in this process.
- 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 through 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 hardly 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.
- N-oxides in which R1 comprises 12 to 24 C atoms and R2 or R3 comprises 1 to 3 C atoms.
- R1 comprises 12 to 24 C atoms
- R2 or R3 comprises 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 ° C is appropriate.
- a temperature of at least 50 ° C is preferred, the upper limit being 200 ° C.
- the 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 wide range of applications covering the concentration range 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 emitter
- 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 produced 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 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.
- Subsequent surfactant treatment of the type proposed can drastically reduce the residual activities or decontamination factors (DF) by 6 to 90 fold for Co-60 and 20 to 350 fold for Am-241.
- DF decontamination factors
- a solution with activity detached from the sample surface was contacted with a cation exchange resin, then mechanically filtered, and then the percent distribution of activity on the exchange resin, filtrate, and filter residue was determined. As a result, it was found that about 95% of the Co-60 and 100% of the Am-241 become bound to the cation exchange resin. Most of the activity can thus be removed from the solution and bonded to the cation exchange resin. This can be supplied to the usual disposal route.
- 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.
Claims (13)
- Procédé de décontamination de surface d'installations nucléaires contaminées par des émetteurs de rayons alpha, qui est réalisé à la suite d'un procédé de décontamination par lequel les couches d'oxyde présentes sur les surfaces ont été éliminées au moins en partie, lors duquel on traite les surfaces à l'aide d'une solution aqueuse, qui contient de l'acide oxalique et un agent tensioactif zwitterionique et/ou cationique, étant utilisés en tant qu'agent tensioactif zwitterionique un acide aminé de la formule générale HOOC-R-NH2 ou un N-oxyde de la formule générale R1(NO)(R2)(R3) avec un reste aliphatique R1 avec de 4 à 24 atomes C et des restes aliphatiques R2, R3 avec chacun de 1 à 10 atomes C, en tant qu'agent tensioactif cationique une amine primaire de la formule générale R-NH2, au moins une partie de la solution étant amenée après son action sur une surface, sur un échangeur d'ions.
- Procédé selon la revendication 1,
caractérisé par
l'utilisation d'un échangeur de cations. - Procédé selon l'une quelconque des revendications précédentes,
caractérisé par
une concentration d'acide oxalique supérieure à 250 ppm. - Procédé selon la revendication 3,
caractérisé par
une concentration d'acide oxalique de 250 ppm à 15000 ppm. - Procédé selon l'une quelconque des revendications précédentes,
caractérisé en ce qu'
il est réalisé à la suite d'une décontamination d'une surface, lors de laquelle on élimine une couche d'oxyde présente sur cette dernière à l'aide d'une solution de nettoyage contenant de l'acide oxalique. - Procédé selon l'une quelconque des revendications précédentes,
caractérisé par
l'utilisation d'une amine avec un reste aliphatique R comprenant de 8 à 24 atomes C. - Procédé selon l'une quelconque des revendications précédentes,
caractérisé par
l'utilisation d'un acide aminé avec un reste aliphatique R avec de 4 à 24 atomes C. - Procédé selon l'une quelconque des revendications précédentes,
caractérisé qu'
il est réalisé avec du N-oxyde de diméthylamino-octadécyle. - Procédé selon l'une quelconque des revendications précédentes,
caractérisé en ce qu'
on travaille avec une concentration d'agent tensioactif supérieure à 20 ppm. - Procédé selon la revendication 9,
caractérisé par
une concentration d'agent tensioactif de 50 ppm à 5000 ppm. - Procédé selon l'une quelconque des revendications précédentes,
caractérisé en ce qu'
il est réalisé à une température supérieure à 30 °C. - Procédé selon la revendication 11,
caractérisé par
une température de 60 °C à 100 °C. - Procédé selon la revendication 1,
caractérisé par
un N-oxyde avec un reste R1 de 12 à 24 atomes C et des restes R2, R3 présentant chacun de 1 à 3 atomes C.
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 EP2188814A2 (fr) | 2010-05-26 |
EP2188814B1 true 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)
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 |
US9947425B2 (en) | 2013-08-14 | 2018-04-17 | Areva Gmbh | Method for reducing the radioactive contamination of the surface of a component used in a nuclear reactor |
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 |
Family Cites Families (15)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
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 |
-
2007
- 2007-08-17 DE DE102007038947A patent/DE102007038947A1/de not_active Withdrawn
-
2008
- 2008-07-16 ES ES08786183T patent/ES2393291T3/es active Active
- 2008-07-16 KR KR1020107005525A patent/KR101182925B1/ko active IP Right Grant
- 2008-07-16 EP EP08786183A patent/EP2188814B1/fr not_active Not-in-force
- 2008-07-16 JP JP2010520517A patent/JP5235216B2/ja not_active Expired - Fee Related
- 2008-07-16 CA CA2695691A patent/CA2695691C/fr not_active Expired - Fee Related
- 2008-07-16 CN CN200880108505.2A patent/CN101809675B/zh not_active Expired - Fee Related
- 2008-07-16 WO PCT/EP2008/059289 patent/WO2009024417A2/fr active Application Filing
-
2009
- 2009-05-27 US US12/472,695 patent/US8702868B2/en not_active Expired - Fee Related
Also Published As
Publication number | Publication date |
---|---|
WO2009024417A2 (fr) | 2009-02-26 |
US20100116288A1 (en) | 2010-05-13 |
EP2188814A2 (fr) | 2010-05-26 |
JP5235216B2 (ja) | 2013-07-10 |
CA2695691A1 (fr) | 2009-02-26 |
US8702868B2 (en) | 2014-04-22 |
KR20100057040A (ko) | 2010-05-28 |
CA2695691C (fr) | 2014-10-21 |
KR101182925B1 (ko) | 2012-09-13 |
JP2010537160A (ja) | 2010-12-02 |
CN101809675B (zh) | 2013-08-21 |
ES2393291T3 (es) | 2012-12-20 |
DE102007038947A1 (de) | 2009-02-26 |
CN101809675A (zh) | 2010-08-18 |
WO2009024417A3 (fr) | 2009-04-23 |
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