EP1449221A1 - Procede de traitement de dechets radioactifs et systeme permettant de mettre ledit procede en oeuvre - Google Patents

Procede de traitement de dechets radioactifs et systeme permettant de mettre ledit procede en oeuvre

Info

Publication number
EP1449221A1
EP1449221A1 EP02767388A EP02767388A EP1449221A1 EP 1449221 A1 EP1449221 A1 EP 1449221A1 EP 02767388 A EP02767388 A EP 02767388A EP 02767388 A EP02767388 A EP 02767388A EP 1449221 A1 EP1449221 A1 EP 1449221A1
Authority
EP
European Patent Office
Prior art keywords
waste
oxidation reactor
water
pressure
fed
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.)
Withdrawn
Application number
EP02767388A
Other languages
German (de)
English (en)
Inventor
Holger Weimer
Karl Heinz Kleinschroth
Johannes Abeln
Manfred Kluth
Helmut Schmieder
Hubert Goldacker
Jan Lamla
Eckhard Dinijus
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
Framatome ANP 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 Framatome ANP GmbH filed Critical Framatome ANP GmbH
Publication of EP1449221A1 publication Critical patent/EP1449221A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F11/00—Treatment of sludge; Devices therefor
    • C02F11/06—Treatment of sludge; Devices therefor by oxidation
    • C02F11/08—Wet air oxidation
    • C02F11/086—Wet air oxidation in the supercritical state
    • 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
    • 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
    • G21F9/32—Processing by incineration
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00—Nature of the contaminant
    • C02F2101/006—Radioactive compounds

Definitions

  • Radioactive waste treatment process and system for carrying out the process
  • the invention relates to a method for treating radioactive waste. It further relates to a system for processing organic waste containing waste from a nuclear facility suitable for carrying out the method.
  • Liquid waste containing organic components can be generated in a nuclear plant, in particular in a nuclear power plant.
  • ion exchange resins are usually used in nuclear plants to remove radioactive isotopes from a water or liquid stream. In this way, especially condensate, circulation or waste water flows are treated.
  • the ion exchange resin used for cleaning can be in bed form (for example as a mixed bed filter) or in the form of
  • Precoat layers are used.
  • cationic and / or anionic ion exchange resins can be used.
  • the respective ion exchange resin can be in powder form as a powder resin.
  • ion exchange resin in the form of small spheres - also known as spherical resin - can also be used.
  • Ion exchange resin used in this way can no longer absorb any more ions after a certain operating period and must therefore be cleaned (regenerated) or discarded and disposed of.
  • the ion exchange resin contains radioactive substances and thus forms radioactive waste containing organic components, so that appropriate safety standards corresponding disposal, conditioning or final storage must be ensured.
  • ion exchange resins conditioned by cementing require a comparatively large intermediate or final storage volume.
  • a volume reduction of waste of this type is usually initially desirable, but on the other hand, special safety standards with regard to reliable final storage capability must also be observed.
  • cementing and subsequent packaging in intermediate or final storage containers is usually provided.
  • such conditioning by cementing or bituminization even leads to an increase in the volume of the waste to be disposed of.
  • the invention is therefore based on the object of specifying a method for treating radioactive waste, which is present in particular in the form of contaminated ion exchange resin, by means of which particularly reliable intermediate or final storage of the waste is made possible with only a small volume requirement. Furthermore, a system for processing organic waste containing waste from a nuclear facility suitable for carrying out the method is to be specified.
  • this object is achieved according to the invention in that the waste to be treated is fed to an oxidation reactor in which wet oxidation of organic components of the waste is carried out under conditions which are supercritical for water.
  • the invention is based on the consideration that a reliable intermediate or final storage for the waste is possible with a small footprint by concentrating the waste on its actually contaminated components or their salt load.
  • the organic constituents formed, for example, by the ion exchange resins or their carrier material should largely be removed from the waste and a separate one adapted to them. disposal.
  • a waste disposal facility which is usually already present in nuclear facilities, should be usable. This is usually designed for the treatment of gaseous waste. Therefore, the organic constituents should be specifically converted into components that can be further processed in a simple manner and removed in this form from the waste.
  • a so-called wet oxidation of the organic constituents in supercritical water is particularly suitable for such a conversion.
  • Supercritical water is water with a pressure above the critical pressure of 221 bar and a temperature above the critical temperature of 374 ° C.
  • the hydrogen bonds are almost completely removed under parameters above these limit values, so that organic or other non-polar substances achieve almost complete miscibility with such supercritical water.
  • This almost complete miscibility with supercritical water also applies to gases such as nitrogen (N 2 ), oxygen (0 2 ) or carbon dioxide (C0 2 ) and to lower hydrocarbons (methane, ethane or the like).
  • Such constituents of the waste that is to say in particular its organic constituents, thus form a single phase with the supercritical water and an oxidizing agent, such as air or oxygen, for example, so that in this state the reaction of the organic constituents by reaction with the oxidizing agent does not is hindered by phase boundaries.
  • the supercritical water in this state has a comparatively high diffusion coefficient with a relatively low viscosity, so that transport processes take place at a particularly high speed.
  • a comparatively good manageability can also be achieved while maintaining high safety requirements by advantageously mixing the waste first with transport water and then feeding this mixture to the oxidation reactor.
  • the supply of water to the oxidation reactor to carry out the wet oxidation is necessary anyway.
  • this water which is required anyway, can also be used as transport water for the waste, in which it is diluted and kept in a pumpable suspension. This makes the waste particularly easy to treat.
  • the reaction rate during wet oxidation can also be influenced by a suitable choice of the mixing ratios or the metering, as a result of which, in particular, overloading of the oxidation reactor and / or soot formation can be reliably avoided.
  • such a conversion of organic constituents can be carried out by wet oxidation in the manner of a self-sustaining reaction if the temperature in the oxidation reactor is set to a value of more than about 480 ° C.
  • an auxiliary fuel is advantageously fed to the oxidation reactor for particularly high flexibility in carrying out the reaction and in particular for influencing reaction rates or degradation rates as required.
  • the reaction can be influenced in a targeted manner and maintained with particularly high reliability.
  • ethanol is expediently used as the auxiliary fuel.
  • air and / or oxygen (0 2 ) is advantageously supplied to the oxidation reactor as an oxidizing agent.
  • the oxidizing agent is preheated in a further advantageous embodiment before it is fed into the oxidation reactor.
  • the stated object is achieved in that the waste can be fed to an oxidation reactor, the pressure housing of which has means for setting a pressure of more than the critical pressure of water and means for setting a temperature of are assigned more than the critical temperature.
  • the system for processing the waste is designed such that its oxidation reactor is suitable for providing comparatively high pressures and comparatively high temperatures in its interior.
  • the oxidation reactor expediently has a pressure housing which is designed to be subjected to an internal pressure of more than 221 bar without appreciably affecting its mechanical stability.
  • the pressure housing is expediently designed, in particular with regard to its wall or its suspension, to be subjected to a temperature of more than 374 ° C.
  • the setting of the temperature inside the oxidation reactor can be influenced by a suitable choice of a feed rate of the waste to be treated and of the oxidizing agent.
  • the system temperature in the Interior of the oxidation reactor can also be influenced by the choice of a suitable feed rate of an auxiliary fuel.
  • the oxidation reactor can advantageously be heated by a number of heating elements arranged on the outer wall of its pressure housing. With such an arrangement, the temperature can thus be set from the outside and independently of the feed of substances into the interior of the oxidation reactor.
  • the ignition of the auxiliary fuel can also be suitably supported by the heating elements, so that in particular the start-up process in the treatment of the waste can be suitably influenced.
  • the treatment system advantageously includes a high-pressure pump connected to a supply line for the waste connected to the oxidation reactor.
  • a feed pressure that is adapted to the actual reaction conditions can already be set in the feed line for the waste.
  • the oxidation reactor is advantageously preceded by a mixer for mixing the waste to be treated with an auxiliary fuel and / or an oxidizing agent.
  • a mixer for mixing the waste to be treated with an auxiliary fuel and / or an oxidizing agent.
  • the oxidation reactor is advantageously designed as a so-called sweat wall reactor, in which the actual reaction zone for carrying out the wet oxidation is spatially decoupled from the surrounding pressure housing via an inner tube.
  • the inner tube is porous, expediently made of ceramic material.
  • the remaining residues essentially correspond to the actual radioactive materials bound in the ion exchange resins, which can thus be sent to a targeted interim or final storage without any significant space requirement.
  • the residues can also be brought into a particularly concentrated form by a subsequent evaporation step.
  • FIG. 1 shows schematically a system for processing waste from a nuclear facility.
  • the system 1 is provided for the treatment of waste A containing organic constituents from a nuclear plant, not shown in detail. Waste A can in particular be used and thus contaminated ion exchange resins. System 1 is designed to treat waste A with the aim of reducing its volume. A transfer into a state capable of being stored in an interim or final storage facility can take place in particular in connection with a subsequent evaporation step.
  • the system 1 is designed for wet oxidation of the organic constituents of the waste A to be treated under conditions which are supercritical for water.
  • the system 1 comprises an oxidation reactor 2, to which the waste A, which is held in a storage container 4 and mixed with transport water, can be fed via a feed line 6.
  • the supply line 6, which can be shut off with a valve 8, into which a high-pressure pump 10 and a preheater 12 are connected are, on the output side, open into a mixer 14 directly upstream of the oxidation reactor 2.
  • a supply container 18 for an auxiliary fuel B and a supply container 22 for an oxidizing agent O are connected to the mixer 14 via a fuel line 16.
  • a high-pressure pump 24 and a preheater 26 are also connected to the fuel line 16.
  • Another preheater 28 is connected in the gas line 20.
  • the oxidation reactor 2 is connected to a phase separator 36 via a waste water line 32, into which a cooler 34 is connected.
  • a control valve 38 is connected, via which the pressure in the oxidation reactor 2 can be adjusted.
  • the control valve 38 further reduces the pressure of the exhaust gas to approximately 1 bar, by means of which it can be supplied to an exhaust system, for example an exhaust system, via a downstream exhaust line 40.
  • the phase separator 36 is connected on the output side to a sewage system, not shown, via a sewage line 44 provided with a control valve 42.
  • the fill level in the phase separator 36 can be set via the control valve 42 and can in particular be kept constant.
  • a sample system 46 is connected to the oxidation reactor 2, to the waste water line 32, to the waste gas line 40 and to the waste water line 44, via which the medium carried in the respective component can be monitored continuously and in particular as a basis for the process control.
  • the oxidation reactor 2 is designed as a so-called sweat wall reactor and comprises a pressure housing 50 in the manner of an outer jacket.
  • An inner tube 52 is arranged inside the tubular pressure housing 50.
  • the inner tube 52 is designed to be porous or perforated, so that overflow on the media side from the intermediate space surrounding the inner tube 52 in a ring between the pressure housing 50 and the inner tube 52 in the inner region of the inner tube 52 is fundamentally possible.
  • the inner tube 52 is designed as a ceramic tube made of a ceramic material with a suitable porosity.
  • a heating device 54 Arranged in the outer area of the pressure housing 50 is a heating device 54, shown only schematically in the figure, which in the exemplary embodiment can be operated electrically via a supply unit (not shown in detail).
  • the heating device 54 comprises a number of heating elements arranged in contact with the pressure housing 50.
  • condensation water SW can also be applied to the annular space formed by the pressure housing 50 and the inner tube 52.
  • a directed flow into the interior of the oxidation reactor 2 can be maintained by supplying condensation water SW. This prevents media-side overflow from the inner region of the inner tube 52 into the space between the pressure housing 50 and the inner tube 52 surrounding it.
  • the condensation water SW can be supplied in the lower region of the oxidation reactor 2 in a cooled form as so-called quench water QW. This serves as a coolant in order to dissipate the heat of reaction occurring in the oxidation reactor 2, it being possible for waste water A 'emerging from the oxidation reactor 2 to be cooled to a temperature of, for example, approximately 250.degree.
  • System 1 is designed for wet oxidation of organic constituents of waste A.
  • the waste A mixed with transport water is introduced into the mixer 14 via the feed line 6 and mixed there with oxidizing agent O, in the exemplary embodiment with air or oxygen 0 2 .
  • oxidizing agent O in the exemplary embodiment with air or oxygen 0 2 .
  • an auxiliary fuel B in the exemplary embodiment ethanol, is also added.
  • the mixture formed in this way is conveyed from the mixer 14 into the interior of the inner tube 52 of the oxidation reactor 2.
  • There are over- critical conditions i.e. an operating pressure of about 300 bar and thus of more than 221 bar and an operating temperature of between about 600 ° C and about 800 ° C and thus more than 374 ° C, set.
  • the operating pressure is adjusted as required via the high-pressure pumps 10, 24 and / or via a compressor 58 assigned to the reservoir 22.
  • the operating temperature is set by independent contributions during the actual wet oxidation, by combustion of the auxiliary fuel B as required and / or by additional ones Heating via the heater 54.
  • the water therein is placed in a supercritical state.
  • the water has a particularly good solubility for comparatively non-polar substances due to the then almost completely disappearing hydrogen bonds.
  • the organic constituents of waste A are dissolved with particularly high effectiveness in the supercritical water thus formed, as are the oxidizing agent O and / or auxiliary fuel B. Since there are no longer any phase boundaries in the supercritical water, an oxidation reaction of the organic constituents of waste A particularly favored with the oxidizing agent O. As a result, the organic constituents of waste A are reacted at a high reaction rate and largely completely with the oxidizing agent O to form carbon dioxide C0 2 and water H 2 0.
  • the oxidation reactor 2 is constructed in the manner mentioned.
  • the inner tube 52 serves to coat the actual reaction zone without the inner tube 52 being exposed to the considerable mechanical loads of the actual pressure housing 50 even as a result of the pressure conditions.
  • the corrosion protection via the inner tube 52 is thus decoupled from the actually mechanically loaded component, namely the pressure vessel 50.
  • the application of condensation water SW to the annular space between the pressure housing 50 and the inner tube 52 takes place with the proviso that a flow through the inner tube 52 from the outside inwards and thus reliably prevent corrosive material entry into this space. By flowing through the inner tube 52, material deposits on its inner wall and thus blockages are also reliably avoided.
  • the condensation water SW is supplied in the lower region of the oxidation reactor 2 in a cooled form as quench water QW. Characterized the reaction mixture is cooled there to a temperature of about 200 ° C to 300 ° C, so that u. a. precipitating inorganic constituents are at least partially dissolved again and thus blockages in the sewage pipe are reliably suppressed.
  • the preheaters 12, 26, 28 serve to keep the temperatures when waste A, oxidizing agent O and auxiliary fuel B enter the oxidation reactor 2 comparatively high in order to minimize the heating-up time in the actual oxidation reactor 2. As a result, a comparatively longer residence time is available for oxidation in the oxidation reactor 2. In addition, soot formation is largely avoided.
  • the preheaters 12, 26, 28 are designed such that the medium flowing through them at each outlet has a temperature of has about 400 ° C. The increase in the operating temperature of these media to the operating temperature provided in the oxidation reactor 2 of approximately 600 ° C. to approximately 800 ° C. can thus be achieved with only limited expenditure.
  • the cooler 34 ensures that the waste water A 'is present with operating parameters that can be used for the phase separator 36, in particular with sufficiently cooled operating temperature. Further wastewater treatment of the wastewater A 'flowing out of the oxidation reactor 2 is thus also made possible.
  • the wet oxidation of organic constituents of the waste A in the oxidation reactor 2 of the system 1 enables a considerable volume reduction of the waste A to be disposed of.
  • the organic constituents of waste A which can make up by far the largest proportion of its volume, are reliably removed and converted into comparatively easy-to-handle substances, namely in particular carbon dioxide (C0 2 ) and water (H 2 0).
  • C0 2 carbon dioxide
  • H 2 0 water
  • Waste water systems a problem-free further treatment possible.
  • the remaining waste on the other hand, can be fed into a reliable intermediate or final storage, especially after a further treatment by evaporation, with only a very small space requirement.
  • the oxidation in the liquid phase means that any cesium which might otherwise pass into the gas phase as a volatile element remains dissolved and thus does not contribute to gaseous waste requiring treatment.
  • a comparatively complex emission control system can thus be dispensed with in the present case.

Landscapes

  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Environmental & Geological Engineering (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Hydrology & Water Resources (AREA)
  • Water Supply & Treatment (AREA)
  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Processing Of Solid Wastes (AREA)
  • Treatment Of Water By Oxidation Or Reduction (AREA)

Abstract

L'invention concerne un procédé permettant de traiter des déchets radioactifs (A) se présentant notamment sous forme de résine échangeuse d'ions contaminée, qui permet d'effectuer un stockage intermédiaire ou final fiable des déchets (A), pour un encombrement volumique particulièrement réduit. A cet effet, selon l'invention, les déchets (A) sont mélangés à de l'eau de transport et le mélange est acheminé jusqu'à un réacteur d'oxydation (2) dans lequel une oxydation par voie humide de constituants organiques des déchets (A) est effectuée, dans des conditions surcritiques pour l'eau (H2O).
EP02767388A 2001-08-17 2002-08-15 Procede de traitement de dechets radioactifs et systeme permettant de mettre ledit procede en oeuvre Withdrawn EP1449221A1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE10140525 2001-08-17
DE10140525A DE10140525A1 (de) 2001-08-17 2001-08-17 Verfahren zur Behandlung von radioaktivem Abfall und System zur Durchführung des Verfahrens
PCT/EP2002/009129 WO2003017288A1 (fr) 2001-08-17 2002-08-15 Procede de traitement de dechets radioactifs et systeme permettant de mettre ledit procede en oeuvre

Publications (1)

Publication Number Publication Date
EP1449221A1 true EP1449221A1 (fr) 2004-08-25

Family

ID=7695848

Family Applications (1)

Application Number Title Priority Date Filing Date
EP02767388A Withdrawn EP1449221A1 (fr) 2001-08-17 2002-08-15 Procede de traitement de dechets radioactifs et systeme permettant de mettre ledit procede en oeuvre

Country Status (4)

Country Link
EP (1) EP1449221A1 (fr)
JP (1) JP2005505756A (fr)
DE (1) DE10140525A1 (fr)
WO (1) WO2003017288A1 (fr)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8017089B2 (en) * 2008-07-25 2011-09-13 Eau-Viron Incorporated Method and apparatus for conducting supercritical wet oxidation reactions contained within a fluid envelope
CN101807444B (zh) * 2010-03-18 2012-02-08 华北电力大学 核电站的细颗粒物脱除装置
DE102021004501A1 (de) 2021-09-04 2023-03-09 Westinghouse Electric Germany Gmbh lonentauscherharzbehandlungssystem und Verfahren dazu

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB9619523D0 (en) * 1996-09-19 1996-10-30 Ferguson Ian G Ferguson cryonator/cryotory
JPH10170694A (ja) * 1996-12-11 1998-06-26 Mitsubishi Heavy Ind Ltd 放射性廃棄物の処理方法

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See references of WO03017288A1 *

Also Published As

Publication number Publication date
WO2003017288A1 (fr) 2003-02-27
DE10140525A1 (de) 2003-03-13
JP2005505756A (ja) 2005-02-24

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