EP2248134B1 - Procédé pour le conditionnement de résines échangeuses d'ions radioactives - Google Patents

Procédé pour le conditionnement de résines échangeuses d'ions radioactives Download PDF

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Publication number
EP2248134B1
EP2248134B1 EP09702004A EP09702004A EP2248134B1 EP 2248134 B1 EP2248134 B1 EP 2248134B1 EP 09702004 A EP09702004 A EP 09702004A EP 09702004 A EP09702004 A EP 09702004A EP 2248134 B1 EP2248134 B1 EP 2248134B1
Authority
EP
European Patent Office
Prior art keywords
water
ion exchange
resin
exchange resin
oxidizing agent
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
Application number
EP09702004A
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German (de)
English (en)
Other versions
EP2248134A1 (fr
Inventor
Rainer Gassen
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 EP2248134A1 publication Critical patent/EP2248134A1/fr
Application granted granted Critical
Publication of EP2248134B1 publication Critical patent/EP2248134B1/fr
Active legal-status Critical Current
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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
    • G21F9/28—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
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
    • G21F9/304—Cement or cement-like matrix

Definitions

  • the invention relates to a method for conditioning radioactive ion exchange resins.
  • Ion exchange resins which are generally present as approximately spherical particles, are used, for example, in the operation of nuclear facilities to clean the coolant of the primary system, ie water. The aim of this cleaning is to avoid unwanted deposits on the surfaces of the primary circuit components, to prevent corrosion and to reduce the build-up of contamination in the primary circuit of the system.
  • Both acid cation exchangers and basic anion exchangers are used in this purification, the former retaining metal cations and the latter anionic compounds, for example metal complexes. Since some of the metals are radionuclides, spent or loaded ion exchangers are radioactive waste and must be disposed of temporarily or permanently.
  • Radioactively contaminated exchange resins also occur in the decontamination of nuclear facilities, for example in the primary circuit decontamination.
  • metal oxide layers present on the surfaces of the primary circuit components are removed by means of decontamination solutions, the solutions being passed through ion exchangers during or after the decontamination in order to remove activity or metal cations contained therein.
  • contaminated ion exchangers which are essentially organic resins with acidic or basic groups, must be conditioned. Conditioning is generally understood to mean the transfer of a radioactive waste into a storable form.
  • spent ion exchange resins are usually dried and after a certain storage period or decay time, in which the radioactivity has dropped to a predetermined limit, for the purpose of storage embedded in a solid matrix, for example, cemented.
  • the embedding of the ion exchange resins in a solid matrix leads to an increase in volume by more than six times the volume of the resin. Due to the large amount of waste arising for the operator of a nuclear power plant considerable costs for the intermediate or final disposal. Therefore, concepts have been developed to reduce the volume of the ion exchange resins.
  • One of these concepts provides for combustion. However, this requires complex filter systems to prevent leakage of radioactivity into the environment. In addition, the combustion does not work very well due to the acidic or basic groups commonly present in the resins.
  • the metals and thus the activity with the aid of acids or alkalis are completely removed from the resins, so that the resins can be reused.
  • the respective acid or alkali is passed over a purely organic, ie neither acidic nor basic groups containing and therefore more easily combustible resin, which binds the metals (and the activity) adsorptive.
  • the complete regeneration of the acidic or basic exchange resins fall considerable Amounts of acid / base secondary waste that needs to be disposed of.
  • the object of the invention is to propose a method for conditioning contaminated ion exchange resins, with which in comparison to the direct embedding in a solid matrix, a volume reduction is connected and can be carried out with little time and material.
  • a method according to claim 1 namely in that the ion exchange resin is mixed with water and with the aid of an oxidizing agent added to the water is at least partially decomposed into water-soluble fragments, wherein the resulting aqueous solution is solidified with a binder the method of reducing the volume of solid resin particles achieved in the reduction of volume consists mainly in the transition from the solid phase in which the resin is in the form of a bulky network of macromolecules to dissolved fragments of this network. Essentially, the process does not require more than one tank for carrying out the resin oxidation and possibly a second tank for the Consolidation.
  • the added oxidizing agent causes the polymer network of the resin, for example, a copolymer of vinylbenzene and divinylbenzene, to be broken to form water-soluble fragments.
  • the water solubility results from the acid or base groups present on the fragments (eg sulfonic acid groups or aminoethyl groups).
  • the oxidation is preferably continued until all or almost all of the resin has dissolved.
  • the exchange resin is treated oxidatively only until it is preferably completely in the form of water-soluble fragments.
  • the resulting amount of carbon dioxide is relatively low.
  • Cement for example Portland cement
  • Portland cement usually contains high proportions of calcium oxide, which together with silicates with the mixing water forms cement hardening hydrates during the setting process. If the water of the mixture to be solidified is acidic, the calcium oxide is dissolved and is no longer available for hydrate formation and thus for cement hardening.
  • a base is added for the neutralization of acids or for raising the pH of the mixture, so that it is slightly acidic to basic at the end.
  • base preferably alkaline earth oxides and hydroxides are used.
  • the oxidation of the ion exchange resins can in principle be carried out with any desired oxidizing agents. Preferably, however, those are used which form no reaction products in their reaction with the resin, which hinder the setting of the cement or other binder. Oxidants that have this property are hydrogen peroxide and ozone were used. Hydrogen peroxide leaves only harmless water, and ozone is reduced to oxygen, which escapes for the most part from the mixture. Resin oxidation produces CO 2 (which mostly escapes) and water.
  • Resins 1 and 2 are relatively low crosslinked polystyrene-based resins having a divinylbenzene content of about 4-6%. Resins 3 and 4 are more crosslinked and have a divinylbenzene content of about 8-12%. The experiments have shown that not all resins are equally degradable. The time required to fully dissolve higher crosslinked resins (Nos. 3 and 4) is greater. Of course, the temperature is also decisive for the duration (see Experiments Nos. 1 and 2). An acceleration of the oxidation can also be achieved by the hydrogen peroxide in higher concentration is added. During oxidation with ozone, it was introduced into the mixture in gaseous form with the aid of a glass frit.

Landscapes

  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Processing Of Solid Wastes (AREA)
  • Treatment Of Water By Ion Exchange (AREA)
  • Separation, Recovery Or Treatment Of Waste Materials Containing Plastics (AREA)

Claims (9)

  1. Procédé de conditionnement d'une résine échangeuse d'ions présentant une contamination radioactive, dans lequel ladite résine est mélangée à de l'eau et décomposée, à l'aide d'un agent oxydant que l'on ajoute à ladite eau, en fragments qui sont au moins partiellement hydrosolubles, la solution aqueuse ainsi obtenue étant solidifiée avec un liant, le cas échéant après une réduction du volume en faisant évaporer de l'eau.
  2. Procédé selon la revendication 1,
    caractérisé en ce que
    l'on utilise, en tant que liant, du ciment.
  3. Procédé selon la revendication 2,
    caractérisé en ce que,
    préalablement à la solidification avec du ciment, on ajoute une base au mélange.
  4. Procédé selon la revendication 3,
    caractérisé en ce que
    l'on utilise, en tant que base, un oxyde ou hydroxyde alcalino-terreux.
  5. Procédé selon l'une des revendications précédentes,
    caractérisé par
    l'utilisation de peroxyde d'hydrogène ou d'ozone en tant qu'agent oxydant.
  6. Procédé selon l'une des revendications précédentes,
    caractérisé en ce que
    le traitement d'oxydation est réalisé à une température élevée, par rapport à la température ambiante.
  7. Procédé selon la revendication 6,
    caractérisé en ce que
    ledit traitement d'oxydation est réalisé à une température comprise entre 80 °C et 100 °C.
  8. Procédé selon l'une des revendications précédentes,
    caractérisé en ce que
    la quantité de l'agent oxydant est choisie de façon à ce que moins de 50 % du carbone contenu dans ladite résine échangeuse est oxydé pour former du dioxyde de carbone et de l'eau.
  9. Procédé selon l'une des revendications 1 à 7,
    caractérisé en ce que
    la quantité de l'agent oxydant est choisie de façon à ce que moins de 20 % du carbone contenu dans ladite résine échangeuse est oxydé pour former du dioxyde de carbone et de l'eau.
EP09702004A 2008-01-17 2009-01-15 Procédé pour le conditionnement de résines échangeuses d'ions radioactives Active EP2248134B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102008005336A DE102008005336A1 (de) 2008-01-17 2008-01-17 Verfahren zur Konditionierung radioaktiver Ionenaustauscherharze
PCT/EP2009/050415 WO2009090209A1 (fr) 2008-01-17 2009-01-15 Procédé pour le conditionnement de résines échangeuses d'ions radioactives

Publications (2)

Publication Number Publication Date
EP2248134A1 EP2248134A1 (fr) 2010-11-10
EP2248134B1 true EP2248134B1 (fr) 2011-06-22

Family

ID=40756569

Family Applications (1)

Application Number Title Priority Date Filing Date
EP09702004A Active EP2248134B1 (fr) 2008-01-17 2009-01-15 Procédé pour le conditionnement de résines échangeuses d'ions radioactives

Country Status (10)

Country Link
US (1) US8372289B2 (fr)
EP (1) EP2248134B1 (fr)
JP (1) JP5543926B2 (fr)
KR (1) KR101183002B1 (fr)
AT (1) ATE514168T1 (fr)
CA (1) CA2711555C (fr)
DE (1) DE102008005336A1 (fr)
ES (1) ES2367238T3 (fr)
TW (1) TWI442414B (fr)
WO (1) WO2009090209A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102018131902B3 (de) * 2018-12-12 2020-02-27 Framatome Gmbh Verfahren zur Konditionierung von Ionenaustauscherharzen und Vorrichtung zur Durchführung des Verfahrens

Family Cites Families (20)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
AT43561B (de) 1909-02-15 1910-08-10 Anton Wrana Getreide-Mahl- und Sichtmaschine.
JPS5341319B2 (fr) * 1971-08-17 1978-11-01
DE2945007A1 (de) 1979-11-08 1981-05-21 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Verfahren zur endlagerreifen, umweltfreundlichen verfestigung von radioaktiven ionenaustauscherharzen
US4437999A (en) 1981-08-31 1984-03-20 Gram Research & Development Co. Method of treating contaminated insoluble organic solid material
JPS5958400A (ja) * 1982-09-28 1984-04-04 日本原子力事業株式会社 放射性イオン交換樹脂の減容固化方法
JPS5998740A (ja) * 1982-11-30 1984-06-07 Mitsui Eng & Shipbuild Co Ltd 使用済イオン交換樹脂の分解処理方法
US4530723A (en) 1983-03-07 1985-07-23 Westinghouse Electric Corp. Encapsulation of ion exchange resins
JPH0232600B2 (ja) * 1983-03-07 1990-07-20 Westinghouse Electric Corp Ionkokanjushisuiseiekikongobutsuosementochunifunyusuruhoho
SE8304278L (sv) 1983-08-04 1985-02-05 Studsvik Energiteknik Ab Forfarande for behandling av anvend, radioaktiv, organisk jonbytarmassa
JPS61165696A (ja) * 1985-01-18 1986-07-26 三菱重工業株式会社 放射性廃棄物処理方法
JPS63158497A (ja) * 1986-08-20 1988-07-01 富士電機株式会社 放射性イオン交換樹脂の分解処理方法
DE3926252A1 (de) * 1989-08-09 1991-02-14 Ghattas Nader Khalil Verfahren und vorrichtung zur zersetzung verbrauchter ionentauscherharze
WO1992003829A1 (fr) * 1990-08-28 1992-03-05 Electric Power Research Institute Procede d'oxydation de matieres organiques sans catalyseur ajoute
FR2678761B1 (fr) * 1991-07-03 1994-07-01 Commissariat Energie Atomique Bloc contenant des resines echangeuses d'ions contaminees et son procede de preparation.
DE69220250T2 (de) * 1992-11-04 1998-01-15 Asea Atom Ab Methode und vorrichtung zur behandlung und entsorgung von verbrauchten ionenaustauscherharz
JP3846820B2 (ja) * 1997-08-20 2006-11-15 株式会社東芝 固体廃棄物処理方法
JP4675521B2 (ja) * 2001-08-15 2011-04-27 日揮株式会社 放射性有機廃棄物の処理方法及び処理装置
JP4414214B2 (ja) * 2003-12-24 2010-02-10 行政院原子能委員會核能研究所 廃イオン交換樹脂の処理方法
EP1564188B1 (fr) 2004-02-13 2006-11-29 Institute of Nuclear Energy Research, Atomic Energy Council Procédé de traitement de résines échangeuses d'ions usées
EP1786000A1 (fr) * 2005-11-09 2007-05-16 AREVA NP GmbH Procédé pour le traitement des résines échangeuses d'ions

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102018131902B3 (de) * 2018-12-12 2020-02-27 Framatome Gmbh Verfahren zur Konditionierung von Ionenaustauscherharzen und Vorrichtung zur Durchführung des Verfahrens
WO2020120143A1 (fr) 2018-12-12 2020-06-18 Framatome Gmbh Procédé de conditionnement de résines échangeuses d'ions et dispositif pour mettre en œuvre le procédé
US12033766B2 (en) 2018-12-12 2024-07-09 Framatome Gmbh Method for conditioning ion exchange resins and apparatus for carrying out the method

Also Published As

Publication number Publication date
DE102008005336A1 (de) 2009-07-30
US8372289B2 (en) 2013-02-12
CA2711555C (fr) 2015-04-14
TW200941502A (en) 2009-10-01
KR101183002B1 (ko) 2012-09-18
ES2367238T3 (es) 2011-10-31
KR20100120155A (ko) 2010-11-12
US20100256435A1 (en) 2010-10-07
JP5543926B2 (ja) 2014-07-09
ATE514168T1 (de) 2011-07-15
JP2011510281A (ja) 2011-03-31
CA2711555A1 (fr) 2009-07-23
TWI442414B (zh) 2014-06-21
WO2009090209A1 (fr) 2009-07-23
EP2248134A1 (fr) 2010-11-10

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