EP2923360A1 - Procédé de décontamination de la surface d'éléments du circuit de refroidissement d'un réacteur nucléaire - Google Patents

Procédé de décontamination de la surface d'éléments du circuit de refroidissement d'un réacteur nucléaire

Info

Publication number
EP2923360A1
EP2923360A1 EP13815419.0A EP13815419A EP2923360A1 EP 2923360 A1 EP2923360 A1 EP 2923360A1 EP 13815419 A EP13815419 A EP 13815419A EP 2923360 A1 EP2923360 A1 EP 2923360A1
Authority
EP
European Patent Office
Prior art keywords
decontamination
aqueous solution
acid
oxide layer
metal ions
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
EP13815419.0A
Other languages
German (de)
English (en)
Other versions
EP2923360B1 (fr
Inventor
Luis Sempere Belda
Jose Pedro MOREIRA DO AMARAL
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
Original Assignee
Areva 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 GmbH filed Critical Areva GmbH
Publication of EP2923360A1 publication Critical patent/EP2923360A1/fr
Application granted granted Critical
Publication of EP2923360B1 publication Critical patent/EP2923360B1/fr
Active 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
    • G21F9/28—Treating solids
    • 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
    • G21F9/30—Processing

Definitions

  • the invention relates to a method for surface decontamination of components of the coolant circuit of a nuclear reactor, ie a pressurized water or boiling water reactor.
  • the core of the coolant circuit is a reactor ⁇ pressure vessel in which nuclear fuel containing fuel elements are arranged.
  • the reactor pressure vessel are usually several ⁇ re cooling loops, each with a coolant pump is ⁇ closed.
  • a pressurized water reactor with temperatures in the range of 300 ° C show even stainless austenitic FeCrNi steels, which, for example, the tube system of cooling loops, Ni alloys, of which, for example, the Austau ⁇ shear tubes of steam generators and other used as coolant pumps, eg cobalt-containing Bautei ⁇ le, some solubility in water.
  • Metal ions liberated from the abovementioned alloys pass with the coolant flow to the reactor pressure vessel, where they are partially converted into radioactive by the neutron radiation prevailing there
  • Nuclides are converted.
  • the nuclides are dispersed by the coolant flow throughout the coolant system and are stored in oxide layers that form on the surfaces of coolant system components during operation.
  • the activated nuclides accumulate in and / or on the oxide layer, so that the radioactivity or the dose rate increases at the Bautei ⁇ len of the coolant system.
  • the oxide layers contained ⁇ th depending on the type of alloy used for a component as the main component iron oxide with divalent and trivalent iron and oxides of other metals, particularly chromium and nickel which are present as alloying constituents in the above-mentioned steels.
  • Nickel is always present in divalent form (Ni 2+ ), chromium in trivalent (Cr 3+ ) form.
  • the oxide layer is containing at chromium components initially oxidatively treated (oxidation step), and subsequent ⁇ hitd the oxide layer under acidic conditions in a so-called.
  • Decontamination step with the aid of an acid which is designated by ⁇ the decontamination or in episodes Dekontklare dissolved.
  • the metal ions passing into the solution in the course of treatment with a deconic acid are removed from the solution by passing them through an ion exchanger.
  • An optionally present after the oxidation step excess oxidant is neutralized or in a reduction ⁇ step by addition of a reducing agent reduces.
  • Removal of metal ions in the decontamination step thus takes place in the absence of an oxidizing agent.
  • the reduction of the excess oxidizing agent may be an independent treatment step, wherein the cleaning solution ⁇ a reducing agent serving for the purpose of reduction, for example, ascorbic acid, citric acid or
  • Oxalic acid is added to the reduction of permanganate ions and manganese dioxide.
  • the reduction of excess oxidizing agent can also be within the decontamination step ⁇ SUC gene, wherein an amount is added to the decontamination of organic acid which is sufficient on one hand to neutralize excess oxidizing agent or reducing and secondly to cause oxide dissolution.
  • a treatment or decontamination cycle comprising the treatment sequence "oxidation step reduction step decontamination step” or "oxidation step decontamination step with simultaneous reduction” is carried out several times in order to ensure adequate decontamination or
  • CORD chemical oxidation, reduction and decontamination
  • the oxidative treatment of the oxide layer is required to solve difficult because chromium III oxide and trivalent chromium-containing mixed oxides, especially spinel in the coming eligible for Dekonta ⁇ mination Dekontklaren.
  • an oxidizing agent such as Ce 4+ , HMn0 4 , H 2 S 2 0 8 , KMn0 4 , KMn0 4 treated with acid or alkali or ozone.
  • the result of this treatment is that Cr-III is oxidized to Cr-VI, which goes into solution as Cr0 4 2 ⁇ .
  • Decontamination step which is always the case when an organic decontamination acid is used, the resulting in the oxidation step Cr-VI, which is present as chromate in the aqueous solution, again reduced to Cr-III.
  • the cleaning solution contains essentially Cr-III, Fe-II, Fe-III, Ni-II and, in addition, radioactive isotopes, e.g. Co-60th These metal ions can be removed from the cleaning solution with an ion exchanger.
  • a commonly used decontamination step is deconic acid
  • Oxalic acid because it can effectively dissolve the oxide layers to be removed from component surfaces.
  • a further disadvantage is that in the course of formation in particular ⁇ sondere of Oxalatniederellen to coprecipitate contained in the aqueous solution radionuclides and thus a Re-contamination of the component surfaces comes.
  • the risk of recontamination is particularly high for components with a large surface to volume ratio. This is especially the case with steam generators which have a very large number of small diameter exchanger tubes.
  • recontamination preferably occurs in zones with low flow.
  • the corresponding metal ions such as Ni in the case of a nickel oxalate precipitate
  • the oxalate in solution, that is not bound in the form of a precipitate, the oxalate in a simple manner, such as before the cleaning solution is passed into a ion exchanger, destroyed in a simple and cost-effective manner ⁇ example with the aid of UV light , ie converted to carbon dioxide and water.
  • the oxide layer is treated with a deconic acid and thereby massive metal ions from the oxide be solved layer, the resulting metal ion concentrations are lower than in conventional decontamination, since at least a portion of the gone in the oxidation step in the metal ions were previously removed, so is no longer in the solution.
  • the risk that the solubility of a metal salt of a Dekontklare (the product of the activities the ⁇ th of the metal cation and the acid anion) is exceeded, and to form a poorly soluble precipitate is thus reduced.
  • nickel and oxalic acid the formation of poorly soluble nickel oxalate precipitates is critical since nickel oxalate has a relatively low solubility ⁇ product.
  • ion exchangers are generally organic in nature, they are sensitive to oxidizing agents, in particular to the preferred used in a process according to the invention permanganic acid or its alkali metal salts, which are very strong oxidizing agent. Therefore, in the case of organic ion exchangers in particular, it is expedient to neutralize an oxidant still present in the aqueous solution with the aid of a reducing agent before the solution is passed over the cation exchanger to remove metal ions.
  • the reducing agent used is the deconic acid used in the subsequent decontamination step. It is advantageous that this acid is already present on site, so that an additional expense, for example, for procurement and storage and for an additional authorization, which would be required when using a different of the deconic acid reducing agent, such as glyoxylic acid, is eliminated.
  • a method according to the invention can be used, for example, for
  • Decontamination of all or part of the coolant ⁇ system of a nuclear reactor, such as a boiling water reactor can be used.
  • FIG. 1 is schematically the
  • Coolant system or the primary circuit of a pressurized water reactor shown. It comprises, in addition to the pressure vessel 1, in which at least in operation a plurality of fuel elements 2 are present, a line system 3, which is connected to the pressure vessel 1, and various installations such as a steam generator 4 and a coolant pump 5.
  • the aim of the cleaning in question or the decontamination is to dissolve an existing on the inner surfaces 7 of the components of the primary circuit oxide layer and to remove their gone into solution components from the aqueous solution.
  • the entire coolant system is filled with an aqueous solution containing, for example, a complex-forming organic acid such as oxalic acid, to which reference will be made hereinafter by way of example.
  • a filling so below is meant a process in which it, therefore forms after switching off power operation after a shutdown of the plant in the coolant system forehand off coolant that at issue aqueous solution, said to imple ⁇ tion the oxidation step, an oxidizing agent, preferably permanganic acid or potassium permanganate, is added.
  • an oxidizing agent preferably permanganic acid or potassium permanganate
  • the oxidation was carried out in acidic solution with permanganic acid as the oxidizing agent with a concentration of about 200 ppm at a temperature of about 90 ° C.
  • permanganic acid as the oxidizing agent with a concentration of about 200 ppm at a temperature of about 90 ° C.
  • the concentration or amount of nickel ions increased to about 6,000 g in about 10 hours and then remained substantially the same.
  • nickel is retained by the cation exchanger, so that its amount or its concentration in the overall system decreases accordingly.
  • the decontamination step (III) was initiated by the addition of oxalic acid.
  • the metered addition was carried out in such a way that an oxalic acid concentration of 2000 ppm was not exceeded in the solution. It can be seen in the diagram that the amount of nickel first increased greatly due to the dissolution of the oxide layer, but then decreased due to the switched cation exchanger 8. If the amount of nickel accumulated in Phase I had not been removed in accordance with the invention, Phase III would have produced a much greater total amount of nickel in the solution of approximately 13,000 grams instead of a nickel of approximately 7,000 grams, resulting in solubility problems and the risk of precipitation ,

Landscapes

  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Food Science & Technology (AREA)
  • Cleaning And De-Greasing Of Metallic Materials By Chemical Methods (AREA)
  • Cleaning By Liquid Or Steam (AREA)
  • Catalysts (AREA)

Abstract

L'invention concerne un procédé de décontamination chimique d'une surface d'un élément métallique du circuit de refroidissement d'une centrale nucléaire qui présente une couche d'oxyde, comprenant au moins une étape d'oxydation dans laquelle la couche d'oxyde est traitée avec une solution aqueuse contenant un agent oxydant, suivie d'une étape de décontamination dans laquelle la couche d'oxyde est traitée avec une solution aqueuse d'un acide de décontamination qui a la propriété de former avec des ions métalliques, en particulier des ions de nickel, un précipité difficilement soluble. Avant la réalisation de l'étape de décontamination, les ions métalliques qui sont arrivés dans la solution pendant l'étape d'oxydation sont enlevés de la solution aqueuse à l'aide d'un échangeur de cations.
EP13815419.0A 2013-01-30 2013-12-11 Procédé de décontamination des composées de circuit de refroidissement d'un réacteur nucléair Active EP2923360B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102013100933.6A DE102013100933B3 (de) 2013-01-30 2013-01-30 Verfahren zur Oberflächen-Dekontamination von Bauteilen des Kühlmittelkreislaufs eines Kernreaktors
PCT/EP2013/076155 WO2014117894A1 (fr) 2013-01-30 2013-12-11 Procédé de décontamination de la surface d'éléments du circuit de refroidissement d'un réacteur nucléaire

Publications (2)

Publication Number Publication Date
EP2923360A1 true EP2923360A1 (fr) 2015-09-30
EP2923360B1 EP2923360B1 (fr) 2016-04-13

Family

ID=49911478

Family Applications (1)

Application Number Title Priority Date Filing Date
EP13815419.0A Active EP2923360B1 (fr) 2013-01-30 2013-12-11 Procédé de décontamination des composées de circuit de refroidissement d'un réacteur nucléair

Country Status (9)

Country Link
US (1) US20150364226A1 (fr)
EP (1) EP2923360B1 (fr)
JP (1) JP6339104B2 (fr)
CN (1) CN104903969B (fr)
AR (1) AR094610A1 (fr)
DE (1) DE102013100933B3 (fr)
ES (1) ES2582377T3 (fr)
TW (1) TWI534833B (fr)
WO (1) WO2014117894A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
RU2773222C1 (ru) * 2021-08-16 2022-05-31 Владимир Дмитриевич Локтионов Способ охлаждения и защиты корпуса ядерного реактора при его нагреве в аварийной ситуации и устройство для его осуществления

Families Citing this family (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR102272949B1 (ko) * 2015-02-05 2021-07-06 프라마톰 게엠베하 원자로의 냉각 시스템에서의 금속 표면 오염 제거 방법
DE102016104846B3 (de) * 2016-03-16 2017-08-24 Areva Gmbh Verfahren zur Behandlung von Abwasser aus der Dekontamination einer Metalloberfläche, Abwasserbehandlungsvorrichtung und Verwendung der Abwasserbehandlungsvorrichtung
MX370759B (es) 2017-01-19 2019-12-13 Framatome Gmbh Metodo para descontaminar superficies metalicas de una instalacion nuclear.
JP6408053B2 (ja) * 2017-03-21 2018-10-17 株式会社東芝 ニッケル基合金除染方法
CN107170503B (zh) * 2017-06-02 2019-04-02 苏州热工研究院有限公司 一种降低在役压水堆核电厂集体剂量的化学清洗方法
DE102017115122B4 (de) * 2017-07-06 2019-03-07 Framatome Gmbh Verfahren zum Dekontaminieren einer Metalloberfläche in einem Kernkraftwerk

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DE4110128A1 (de) * 1990-04-09 1991-11-07 Westinghouse Electric Corp Dekontamination von radioaktiv verseuchten metallen
FR2699936B1 (fr) * 1992-12-24 1995-01-27 Electricite De France Procédé de dissolution d'oxydes déposés sur un substrat métallique.
US6147274A (en) * 1996-11-05 2000-11-14 Electric Power Research Insitute Method for decontamination of nuclear plant components
JP3866402B2 (ja) * 1998-02-17 2007-01-10 株式会社東芝 化学除染方法
EP1054413B1 (fr) * 1999-05-13 2013-07-17 Kabushiki Kaisha Toshiba Procédé et appareil pour la décontamination d'éléments d'installation de manipulation de matériels radioactifs
JP3977963B2 (ja) * 1999-09-09 2007-09-19 株式会社日立製作所 化学除染方法
JP2003098294A (ja) * 2001-09-27 2003-04-03 Hitachi Ltd オゾンを用いた除染方法及びその装置
KR100724710B1 (ko) * 2002-11-21 2007-06-04 가부시끼가이샤 도시바 방사화 부품의 화학적 오염제거 시스템 및 방법
BRPI0611248A2 (pt) * 2005-11-29 2009-07-07 Areva Np Gmbh processo para a descontaminação de uma superfìcie, que apresenta uma camada de óxido, de um componente ou de um sistema de uma usina com tecnologia nuclear
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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
RU2773222C1 (ru) * 2021-08-16 2022-05-31 Владимир Дмитриевич Локтионов Способ охлаждения и защиты корпуса ядерного реактора при его нагреве в аварийной ситуации и устройство для его осуществления

Also Published As

Publication number Publication date
CN104903969B (zh) 2017-11-24
CN104903969A (zh) 2015-09-09
TWI534833B (zh) 2016-05-21
AR094610A1 (es) 2015-08-12
US20150364226A1 (en) 2015-12-17
WO2014117894A1 (fr) 2014-08-07
EP2923360B1 (fr) 2016-04-13
TW201442040A (zh) 2014-11-01
DE102013100933B3 (de) 2014-03-27
ES2582377T3 (es) 2016-09-12
JP6339104B2 (ja) 2018-06-06
JP2016504601A (ja) 2016-02-12

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