WO1996032729A1 - Procede de traitement de combustible oxyde nucleaire - Google Patents

Procede de traitement de combustible oxyde nucleaire Download PDF

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Publication number
WO1996032729A1
WO1996032729A1 PCT/GB1996/000872 GB9600872W WO9632729A1 WO 1996032729 A1 WO1996032729 A1 WO 1996032729A1 GB 9600872 W GB9600872 W GB 9600872W WO 9632729 A1 WO9632729 A1 WO 9632729A1
Authority
WO
WIPO (PCT)
Prior art keywords
carbonate
oxide
uranium
fuel
salt
Prior art date
Application number
PCT/GB1996/000872
Other languages
English (en)
Inventor
Mark Fields
Peter David Wilson
Original Assignee
British Nuclear Fuels Plc
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 British Nuclear Fuels Plc filed Critical British Nuclear Fuels Plc
Publication of WO1996032729A1 publication Critical patent/WO1996032729A1/fr

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Classifications

    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01GCOMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G43/00Compounds of uranium
    • C01G43/01Oxides; Hydroxides
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B60/00Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
    • C22B60/02Obtaining thorium, uranium, or other actinides
    • C22B60/0204Obtaining thorium, uranium, or other actinides obtaining uranium
    • C22B60/0213Obtaining thorium, uranium, or other actinides obtaining uranium by dry processes
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B60/00Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
    • C22B60/02Obtaining thorium, uranium, or other actinides
    • C22B60/04Obtaining plutonium
    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21CNUCLEAR REACTORS
    • G21C19/00Arrangements for treating, for handling, or for facilitating the handling of, fuel or other materials which are used within the reactor, e.g. within its pressure vessel
    • G21C19/42Reprocessing of irradiated fuel
    • G21C19/44Reprocessing of irradiated fuel of irradiated solid fuel
    • G21C19/48Non-aqueous processes
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00Energy generation of nuclear origin
    • Y02E30/30Nuclear fission reactors
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02WCLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00Technologies for solid waste management
    • Y02W30/50Reuse, recycling or recovery technologies

Definitions

  • the present invention relates to the processing of irradiated oxide nuclear fuel material.
  • Nuclear fuels discharged after irradiation in a nuclear
  • salt processing techniques is that the molten salt materials are highly corrosive to plant and waste containers and are also, in the case of fluorides, highly
  • a method for the processing of oxide nuclear fuel containing uranium including the step of reacting the oxide with a fused alkali metal carbonate to produce a compound which may be further processed so as to extract at
  • the carbonate may comprise sodium carbonate, Na,C0 3 ;
  • Mixtures may be chosen on the basis of their
  • Such chemicals may include an oxidising agent such as
  • air or oxygen may be passed
  • the molten carbonate salt may also contain sodium hydroxide or other alkali compound as appropriate in order to assist
  • the molten carbonate salt may also include a proportion of alkali metal halide such as sodium chloride or potassium
  • fluoride for example, in order to assist dissolution of the oxide fuel into the carbonate.
  • Dissolution of the irradiated fuel material may be enhanced by a further processing step of initially oxidising the fuel oxide to convert it into uranium oxide powder of composition U 3 0 3 or U0 3 by known techniques.
  • the mixture may be further processed so as to remove the uranium, plutonium and neptunium, if present, from the mixture. Such further processing may normally
  • a first electrolysis stage may be to remove at least a
  • Irradiated thermal reactor fuel normally has in the region of 1% plutonium therein whereas new fuel may have about 6% plutonium or more therein. Therefore, electrolysis may preferably be continued so as to increase the relative proportion of plutonium to uranium to substantially above 6%.
  • a second electrolysis stage may employ a different cathode so as to allow the extraction of at least the plutonium, the plutonium and most of the remaining uranium migrating thereto and alloying therewith.
  • a cathode may comprise, for example, molten cadmium metal.
  • the resulting cadmium/ plutonium/ uranium (/neptunium) cathode is removed and the unwanted cadmium removed, for example, by distilling the cadmium off.
  • the remaining fuel metal elements being further processed into the desired final fuel oxide
  • the wastes produced are less mobile in a disposal environment than the alkali metal halides of the prior art and are thus easier to dispose of.
  • the method of the present invention may be operated as a batch process, the process employing a first step of making a required fused carbonate salt mixture and adding the irradiated fuel thereto in the required proportion to achieve at least partial dissolution of the fuel oxide therein; a second step may be the first electrolysis stage
  • a third step may be the second electrolysis stage as described above,- and, a fourth step may include the further processing of the resulting uranium and/or plutonium and any other metal by-products into the final desired products such as U0 2 powder or PuO, powder for the manufacture of new fuel rods for example.
  • the first and second electrolysis stages may be carried out
  • each stage, or separate electrolysis cells may be employed
  • the carbonate salt may be melted and maintained molten by
  • the molten cadmium cathode may be maintained molten by the
  • Such oxides may include silica and phosphorus
  • Figure 1 shows a flow diagram of an embodiment of a
  • Figure 2 shows a schematic cross section of an electrolysis cell for carrying out a first electrolysis stage,- and
  • Figure 3 which shows a schematic cross section of an electrolysis cell for carrying out a second electrolysis stage.
  • Irradiated fuel rods are first chopped into
  • breached fuel rods are added to the fused carbonate mixture
  • molten metal cathode such as cadmium
  • the extracted plutonium/ uranium/ neptunium/ cadmium alloy from 22 is then processed by heating and distilling off the cadmium (24) to leave the required product (26) .
  • Figure 2 shows a schematic cross section through an
  • the cell for carrying out a first electrolysis stage.
  • the cell comprises a vessel 40 having therein a
  • fused carbonate salt mixture 42 in which an irradiated oxide fuel has been reacted so as to achieve at least partial dissolution.
  • An anode 44 and cathode 46 are provided together with a power supply and control apparatus 48.
  • Heaters 50 are provided to melt and maintain molten the salt/oxide fuel mixture 42. Electrolysis of the mixture 42 results in uranium or uranium oxide 52 being deposited on
  • the cathode 46 so as to deplete the uranium content in the mixture 42. If all of the oxide fuel was not initially reacted or dissolved in the fused carbonate salt, as the uranium content drops during electrolysis, more of the oxide fuel will react with the salt mixture or reacted but
  • the initial reaction of the oxide fuel with the carbonate and oxygen, either from an oxide in the fused salt mixture or from air or oxygen passed through the molten salt may be typically described by the reaction:
  • reaction In the first electrolysis stage to extract uranium, the reaction may be described by:
  • Figure 3 shows a schematic cross section through an electrolysis cell for carrying out a second electrolysis stage of the method according to the present invention.
  • a cell comprises a vessel 70 having heaters 72 to maintain molten a salt mixture 74 resulting from the first electrolysis stage as described above with reference to
  • An anode 78 and power supply and control apparatus 80 are provided.
  • plutonium ions and uranium ions (and neptunium ions if present) migrate to the molten cadmium cathode and alloy therewith.
  • the cadmium cathode is removed and the cadmium metal removed by distilling off at high temperature to leave behind the required metals which may be further processed according to known techniques to produce new fuel rods.
  • the reaction to extract plutonium from the fused salt during the second electrolysis stage may be of the form:

Landscapes

  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Organic Chemistry (AREA)
  • Geology (AREA)
  • Physics & Mathematics (AREA)
  • Environmental & Geological Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Inorganic Chemistry (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Electrolytic Production Of Metals (AREA)

Abstract

Cette invention concerne un procédé destiné au traitement de combustible oxyde nucléaire contenant de l'uranium, ce procédé consistant à faire réagir l'oxyde avec un carbonate fondu de métal alcalin pour obtenir un composé qui peut subir un traitement ultérieur en vue de l'extraction d'au moins une partie de l'uranium et d'autres produits dérivés.
PCT/GB1996/000872 1995-04-12 1996-04-09 Procede de traitement de combustible oxyde nucleaire WO1996032729A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB9507644.4 1995-04-12
GB9507644A GB9507644D0 (en) 1995-04-12 1995-04-12 Method of processing oxide nuclear fuel

Publications (1)

Publication Number Publication Date
WO1996032729A1 true WO1996032729A1 (fr) 1996-10-17

Family

ID=10772980

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/GB1996/000872 WO1996032729A1 (fr) 1995-04-12 1996-04-09 Procede de traitement de combustible oxyde nucleaire

Country Status (2)

Country Link
GB (1) GB9507644D0 (fr)
WO (1) WO1996032729A1 (fr)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO1999041752A1 (fr) * 1998-02-11 1999-08-19 British Nuclear Fuels Plc Retraitement de combustible nucleaire
GB2341396A (en) * 1998-09-11 2000-03-15 Toshiba Kk Molten salt electrolysis of nuclear waste
GB2352729A (en) * 1998-09-11 2001-02-07 Toshiba Kk Molten salt electrolysis of nuclear waste including filtering
US6379634B1 (en) 1996-08-02 2002-04-30 British Nuclear Fuels Plc Ionic liquids as solvents
RU2591215C1 (ru) * 2015-05-06 2016-07-20 Федеральное государственное бюджетное образовательное учреждение высшего профессионального образования "Российский химико-технологический университет имени Д.И. Менделеева" (РХТУ им. Д.И. Менделеева) Способ переработки облученного ядерного топлива
RU2619583C1 (ru) * 2016-09-01 2017-05-17 Федеральное Государственное Унитарное Предприятие "Горно - Химический Комбинат" (Фгуп "Гхк") Способ окислительной обработки (волоксидации) облученного ядерного топлива

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1108042A (en) * 1964-06-10 1968-03-27 Euratom Process for reprocessing nuclear fuels
NL7006446A (fr) * 1969-05-27 1970-12-01
GB1226198A (fr) * 1967-12-21 1971-03-24
FR2181883A1 (fr) * 1972-04-27 1973-12-07 Agip Nucleare Spa
BE815189A (fr) * 1974-05-17 1974-09-16 Procede de conditionnement de combustible nucleaire irradie

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1108042A (en) * 1964-06-10 1968-03-27 Euratom Process for reprocessing nuclear fuels
GB1226198A (fr) * 1967-12-21 1971-03-24
NL7006446A (fr) * 1969-05-27 1970-12-01
FR2181883A1 (fr) * 1972-04-27 1973-12-07 Agip Nucleare Spa
BE815189A (fr) * 1974-05-17 1974-09-16 Procede de conditionnement de combustible nucleaire irradie

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
FUJINO ET AL.: "Reaction of Lithium and Sodium Nitrates and Carbonates with Uranium Oxides", JOURNAL OF NUCLEAR MATERIALS, vol. 116, 1983, AMSTERDAM, NL, pages 157 - 165, XP000576745 *
PIERCE R D ET AL: "PROGRESS IN THE PYROCHEMICAL PROCESSING OF SPENT NUCLEAR FUELS", JOM, vol. 45, no. 2, 1 February 1993 (1993-02-01), WARRENDALE US, pages 40 - 44, XP000344910 *

Cited By (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6379634B1 (en) 1996-08-02 2002-04-30 British Nuclear Fuels Plc Ionic liquids as solvents
WO1999041752A1 (fr) * 1998-02-11 1999-08-19 British Nuclear Fuels Plc Retraitement de combustible nucleaire
GB2341396A (en) * 1998-09-11 2000-03-15 Toshiba Kk Molten salt electrolysis of nuclear waste
GB2352729A (en) * 1998-09-11 2001-02-07 Toshiba Kk Molten salt electrolysis of nuclear waste including filtering
GB2341396B (en) * 1998-09-11 2001-05-23 Toshiba Kk Method of treating waste from nuclear fuel handling facility and apparatus for carrying out the same
US6299748B1 (en) 1998-09-11 2001-10-09 Kabushiki Kaisha Toshiba Method and apparatus of treating waste from nuclear fuel handling facility
GB2352729B (en) * 1998-09-11 2002-04-24 Toshiba Kk Method of treating waste from nuclear fuel handling facility and apparatus for carrying out the same
US6736951B2 (en) 1998-09-11 2004-05-18 Kabushiki Kaisha Toshiba Method of treating waste from nuclear fuel handling facility and apparatus for carrying out the same
RU2591215C1 (ru) * 2015-05-06 2016-07-20 Федеральное государственное бюджетное образовательное учреждение высшего профессионального образования "Российский химико-технологический университет имени Д.И. Менделеева" (РХТУ им. Д.И. Менделеева) Способ переработки облученного ядерного топлива
RU2619583C1 (ru) * 2016-09-01 2017-05-17 Федеральное Государственное Унитарное Предприятие "Горно - Химический Комбинат" (Фгуп "Гхк") Способ окислительной обработки (волоксидации) облученного ядерного топлива

Also Published As

Publication number Publication date
GB9507644D0 (en) 1995-06-14

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