EP2923360B1 - Procédé de décontamination des composées de circuit de refroidissement d'un réacteur nucléair - Google Patents

Procédé de décontamination des composées de circuit de refroidissement d'un réacteur nucléair Download PDF

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Publication number
EP2923360B1
EP2923360B1 EP13815419.0A EP13815419A EP2923360B1 EP 2923360 B1 EP2923360 B1 EP 2923360B1 EP 13815419 A EP13815419 A EP 13815419A EP 2923360 B1 EP2923360 B1 EP 2923360B1
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EP
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Prior art keywords
decontamination
acid
aqueous solution
metal ions
oxide layer
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EP13815419.0A
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German (de)
English (en)
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EP2923360A1 (fr
Inventor
Luis Sempere Belda
Jose Pedro MOREIRA DO AMARAL
Christian Topf
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Areva GmbH
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Areva GmbH
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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
    • G21F9/001—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, that is, 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.
  • At the reactor pressure vessel several cooling loops are usually connected, each with a coolant pump.
  • 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 the cooling loops, Ni alloys, of which, for example, the exchanger tubes of steam generators and others about used for coolant pumps, eg cobalt-containing components, a certain 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 nuclides by the neutron radiation prevailing there.
  • 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 oxide layers contain iron oxide with di- and tri-valent iron and oxides of other metals, especially chromium and nickel, which are present as alloying constituents in the steels mentioned above, depending on the type of alloy used for a component.
  • Nickel is always present in divalent form (Ni 2+ ), chromium in trivalent (Cr 3+ ) form.
  • the oxide layer is first treated oxidatively in the case of components containing chromium (oxidation step) and then the oxide layer is dissolved under acidic conditions in a so-called decontamination step with the aid of an acid, which is referred to below as decontamination or deconic acid.
  • decontamination or deconic acid 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 excess of oxidizing agent optionally present after the oxidation step is neutralized or reduced in a reduction step by addition of a reducing agent.
  • the dissolution of the oxide layer or the dissolution of metal ions in the decontamination step thus takes place in the absence of an oxidizing agent.
  • the reduction of the excess oxidant may be an independent treatment step, wherein the cleaning solution is metered into a reduction agent serving for the purpose of reduction, for example ascorbic acid, citric acid or oxalic acid for the reduction of permanganate ions and manganese dioxide.
  • a reduction agent serving for the purpose of reduction
  • the reduction of excess oxidizing agent can also take place in the context of the decontamination step, wherein an amount of organic decontamination acid is added which is sufficient to neutralize or reduce excess oxidant on the one hand and to cause oxide dissolution on the other hand.
  • a treatment or decontamination cycle comprising the treatment sequence "Oxidation Step Reduction Step Decontamination Step” or “Oxidation Step Decontamination Step with Simultaneous Reduction” is performed several times to achieve sufficient decontamination or reduction of the radioactivity of the component surfaces.
  • Decontamination methods of the type described above are known, for example, under the name CORD (chemical oxidation, reduction and decontamination).
  • the oxidative treatment of the oxide layer is necessary because chromium-III oxides and trivalent chromium-containing mixed oxides, especially of the spinel type, are difficult to dissolve in the decontaminates in question for decontamination.
  • an oxidizing agent such as Ce 4+ , HMnO 4 , H 2 S 2 O 8 , KMnO 4 , KMnO 4 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 CrO 4 2- .
  • 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.
  • Deconic acid which is commonly used in the decontamination step, is oxalic acid because it effectively dissolves the oxide layers to be removed from component surfaces.
  • deconic acids especially oxalic acid
  • oxalate precipitates with bivalent metal ions such as Ni 2+ , Fe 2+ , and Co 2+ sparingly soluble precipitates, in the case of oxalic acid, to which reference is made below.
  • the said precipitates can be distributed throughout the coolant system, depositing on the inner surfaces of pipelines and components, such as steam generators.
  • the rainfall complicates the entire process implementation.
  • a further disadvantage is that in the course of the formation of, in particular, oxalate precipitates for coprecipitation of radionuclides contained in the aqueous solution and thus to 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.
  • a further disadvantage of the formation of oxalate and other precipitates is that they can clog filter devices, such as the filter upstream of an ion exchanger and sieve trays or the protection filters of circulating pumps.
  • a further disadvantage arises when a treatment cycle comprising an oxidation step and a decontamination step described above is repeated, that is to say when a renewed oxidation step follows a deconstruction step. If precipitation has occurred in the previous decontamination step, the corresponding metal ions, such as Ni in the case of a nickel oxalate precipitate, can not be removed from the cleaning solution by means of ion exchangers.
  • the oxalate residue of the precipitates is oxidized to carbon dioxide and water, thereby consuming oxidizing agent uselessly.
  • 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 an ion exchanger, destroyed in a simple and cost-effective manner, for example by means of UV light, ie converted to carbon dioxide and water.
  • This object is achieved in a decontamination process of the type mentioned above by metal ions that have passed into the aqueous solution during the oxidation step, be removed before performing the decontamination step, ie before the addition of an organic deconic acid, using a cation exchanger from the solution.
  • the procedure is advantageously such that the aqueous solution is passed through a cation exchanger.
  • the removal of nickel is particularly advantageous since it forms salts or precipitates which are particularly sparingly soluble with organic acids.
  • the oxide layer is treated with a deconic acid and solid metal ions from the oxide layer can be solved, 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 have been removed before, so is no longer in the solution.
  • the risk of the solubility product of a metal salt of a deconic acid (the product of the activities of the metal cation and the acid anion) being exceeded and a sparingly soluble precipitate forming is thus reduced.
  • the formation of sparingly soluble nickel oxalate precipitates is critical because 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 their 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 on site, so that an additional effort for example for procurement and warehousing and for an additional authorization, which would be when using a different of the deconic acid reducing agent, such as glyoxylic required.
  • An inventive method 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.
  • Fig. 1 schematically the coolant system and the primary circuit of a pressurized water reactor is 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 conduit 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 this is also to be understood as a procedure in which the coolant present after switching off the power operation, ie after the shutdown of the system in the coolant system forms the aqueous solution in question, this being used to carry out 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.
  • oxalic acid as reducing agent was metered into the aqueous solution in a slightly more than stoichiometric amount to neutralize unconsumed permanganic acid.
  • nickel is retained by the cation exchanger, so that its present in the total system amount or its concentration 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 present invention, Phase III, rather than a 7,000 gram nickel, would have resulted in a substantially greater total nickel in the solution of approximately 13,000 grams, resulting in solubility problems and the risk of precipitation ,

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  • 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)

Claims (6)

  1. Procédé de décontamination chimique d'une surface d'un composant métallique du système de refroidissement d'une centrale nucléaire présentant 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 d'oxydation, et une étape subséquente 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 un précipité difficilement soluble avec des ions métalliques, en particulier des ions de nickel, caractérisé en ce que, avant la réalisation de l'étape de décontamination, on retire de la solution aqueuse les ions métalliques, mis en solution pendant l'étape d'oxydation, à l'aide d'un échangeur de cations.
  2. Procédé selon la revendication 1, caractérisé en ce que, avant le retrait des ions métalliques, on procède à une étape de réduction dans laquelle on neutralise un agent d'oxydation présent dans la solution aqueuse à l'aide d'un agent de réduction.
  3. Procédé selon la revendication 2, caractérisé en ce que l'agent de réduction utilisé est l'acide de décontamination employé dans l'étape de décontamination subséquente.
  4. Procédé selon l'une quelconque des revendications précédentes, caractérisé en qu'on fait passer au moins une partie de la solution aqueuse par un échangeur d'ions et de cations tout en retirant les ions métalliques contenus dans la solution aqueuse.
  5. Procédé selon l'une quelconque des revendications précédentes, caractérisé en qu'on utilise de l'acide permanganique ou un sel de l'acide permanganique à l'étape d'oxydation.
  6. Procédé selon l'une quelconque des revendications précédentes par l'utilisation d'acide oxalique comme acide de décontamination.
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 EP2923360A1 (fr) 2015-09-30
EP2923360B1 true EP2923360B1 (fr) 2016-04-13

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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
WO2018134067A1 (fr) 2017-01-19 2018-07-26 Framatome Gmbh Procédé de décontamination de surfaces métalliques d'une installation nucléaire

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP6796587B2 (ja) * 2015-02-05 2020-12-09 フラマトム ゲゼルシャフト ミット ベシュレンクテル ハフツング 原子炉の冷却システムで金属表面を除染する方法
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
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

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US4587043A (en) * 1983-06-07 1986-05-06 Westinghouse Electric Corp. Decontamination of metal surfaces in nuclear power reactors
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FR2699936B1 (fr) * 1992-12-24 1995-01-27 Electricite De France Procédé de dissolution d'oxydes déposés sur un substrat métallique.
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JP3977963B2 (ja) * 1999-09-09 2007-09-19 株式会社日立製作所 化学除染方法
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KR100724710B1 (ko) * 2002-11-21 2007-06-04 가부시끼가이샤 도시바 방사화 부품의 화학적 오염제거 시스템 및 방법
CN101199026B (zh) * 2005-11-29 2012-02-22 阿利发Np有限公司 对核技术设施的部件或系统的含氧化层表面去污的方法
DE102009002681A1 (de) * 2009-02-18 2010-09-09 Areva Np Gmbh Verfahren zur Dekontamination radioaktiv kontaminierter Oberflächen
DE102009047524A1 (de) * 2009-12-04 2011-06-09 Areva Np Gmbh Verfahren zur Oberflächen-Dekontamination

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2018134067A1 (fr) 2017-01-19 2018-07-26 Framatome Gmbh Procédé de décontamination de surfaces métalliques d'une installation nucléaire
US11443863B2 (en) 2017-01-19 2022-09-13 Framatome Gmbh Method for decontaminating metal surfaces of a nuclear facility

Also Published As

Publication number Publication date
AR094610A1 (es) 2015-08-12
TW201442040A (zh) 2014-11-01
TWI534833B (zh) 2016-05-21
CN104903969B (zh) 2017-11-24
JP6339104B2 (ja) 2018-06-06
DE102013100933B3 (de) 2014-03-27
WO2014117894A1 (fr) 2014-08-07
EP2923360A1 (fr) 2015-09-30
CN104903969A (zh) 2015-09-09
JP2016504601A (ja) 2016-02-12
US20150364226A1 (en) 2015-12-17
ES2582377T3 (es) 2016-09-12

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