US20090294299A1 - Spent fuel reprocessing method - Google Patents

Spent fuel reprocessing method Download PDF

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Publication number
US20090294299A1
US20090294299A1 US12/470,226 US47022609A US2009294299A1 US 20090294299 A1 US20090294299 A1 US 20090294299A1 US 47022609 A US47022609 A US 47022609A US 2009294299 A1 US2009294299 A1 US 2009294299A1
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United States
Prior art keywords
electrolysis
cathode
precipitate
oxalic acid
dissolving
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Abandoned
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US12/470,226
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English (en)
Inventor
Koji MIZUGUCHI
Reiko Fujita
Kouki FUSE
Hitoshi Nakamura
Kazuhiro Utsunomiya
Akihiro KAWABE
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Toshiba Corp
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Toshiba Corp
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Assigned to KABUSHIKI KAISHA TOSHIBA reassignment KABUSHIKI KAISHA TOSHIBA ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: FUJITA, REIKO, FUSE, KOUKI, KAWABE, AKIHIRO, MIZUGUCHI, KOJI, NAKAMURA, HITOSHI, UTSUNOMIYA, KAZUHIRO
Publication of US20090294299A1 publication Critical patent/US20090294299A1/en
Abandoned legal-status Critical Current

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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C19/00—Arrangements 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
    • G21C19/42—Reprocessing of irradiated fuel
    • G21C19/44—Reprocessing of irradiated fuel of irradiated solid fuel
    • G21C19/46—Aqueous processes, e.g. by using organic extraction means, including the regeneration of these means
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C1/00—Electrolytic production, recovery or refining of metals by electrolysis of solutions
    • C25C1/22—Electrolytic production, recovery or refining of metals by electrolysis of solutions of metals not provided for in groups C25C1/02 - C25C1/20
    • 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
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C3/00—Electrolytic production, recovery or refining of metals by electrolysis of melts
    • C25C3/34—Electrolytic production, recovery or refining of metals by electrolysis of melts of metals not provided for in groups C25C3/02 - C25C3/32
    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00—Energy generation of nuclear origin
    • Y02E30/30—Nuclear fission reactors
    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00—Technologies related to metal processing
    • Y02P10/20—Recycling
    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00—Technologies for solid waste management
    • Y02W30/50—Reuse, recycling or recovery technologies

Definitions

  • the present invention relates to a spent fuel reprocessing method comprising a step of collecting uranium (U), plutonium (Pu) and minor actinides (MA) from spent oxide nuclear fuel.
  • the Purex process is a known typical process for reprocessing spent fuel produced from nuclear power plants so as to refine and collect useful substances contained in the spent fuel in order to reutilize them as fuel and isolate unnecessary fission products.
  • Spent fuel contains alkali metal (AM) elements, alkaline-earth metal (AEM) elements and platinum group elements as fission products (FP) besides transuranic elements (TRU) such as uranium and plutonium.
  • AM alkali metal
  • AEM alkaline-earth metal
  • FP fission products
  • TRU transuranic elements
  • the high level liquid waste produced from a Purex process contains U and Pu to a small extent and minor actinides (Np: Neptunium, Am: Americium, Cm: Curium, etc.) to a large extent.
  • the aqua-pyro process is known to collect such transuranic elements (Pu and minor actinides) in combination by applying a technique of oxalic acid precipitation—conversion to chloride—molten salt electrolysis to high-level liquid waste (Patent Documents 1 and 2: Japanese Patent No. 2,809,819 Publication and Japanese Patent No. 3,319,657 Publication). The entire content of which is incorporated herein by reference.
  • Pu and U are made to accompany minor actinides and collected in combination with each other. In other words, Pu is not collected alone by itself.
  • a spent fuel reprocessing method comprising: a disassembly/shear step of disassembling and shearing spent oxide nuclear fuel; a dissolution step of dissolving the fuel subjected to the disassembly/shear step in nitric acid solution; an electrolysis/valence adjustment step of reducing plutonium to trivalent, maintaining the pentavalent of neptunium for the fuel subjected to the dissolution step; a uranium extraction step of collecting uranium oxide by bringing the fuel subjected to the electrolysis/valence adjustment step into contact with organic solvent and extracting hexavalent uranium by means of an extraction agent; an oxalic acid precipitation step of causing the minor actinides and the fissure products remaining in the nitric acid solution after the uranium extraction step to precipitate together as oxalic acid precipitate by means of an oxalic acid precipit
  • a spent fuel reprocessing method comprising: a disassembly/shear step of disassembling and shearing spent oxide nuclear fuel; a dissolution step of dissolving the fuel subjected to the disassembly/shear step in nitric acid solution; an electrolysis/valence adjustment step of reducing plutonium and neptunium respectively to trivalent and pentavalent for the fuel subjected to the dissolution step; a uranium extraction step of collecting uranium oxide by bringing the fuel subjected to the electrolysis/valence adjustment step into contact with organic solvent and extracting hexavalent uranium by means of an extraction agent; an oxalic acid precipitation step of causing the minor actinides and the fissure products remaining in the nitric acid solution after the uranium extraction step to precipitate together as oxalic acid precipitate by means of an oxalic acid precipitation method; an oxidation/
  • the present invention it is possible to isolate most of the uranium from spent fuel solution and collect it as light water reactor fuel, while it is possible to collect Pu and minor actinides with U so as to make them utilizable as metal fuel for a fast reactor.
  • Pu is not collected alone by itself and Pu and minor actinides are collected with U, the present invention can ensure a high degree of nuclear non-proliferability.
  • FIG. 1 is a flowchart of spent fuel reprocessing method according to a first embodiment of the present invention
  • FIG. 2 is a schematic sectional elevational view of an apparatus that can be employed for an electrolysis/valence adjustment step of spent fuel reprocessing method according to the first embodiment of the present invention
  • FIG. 3 is a graph showing some of the results of measurement of the initial value of the electrode potential and that of the current density in the electrolysis/valence adjustment step of spent fuel reprocessing method according to the first embodiment of the present invention
  • FIG. 4 is a graph showing some of the results of measurement of the change with time of the current density when the electrolysis potential is held to ⁇ 100 mV relative to a reference electrode, which is a silver/silver salt electrode, in the electrolysis/valence adjustment step of spent fuel reprocessing method according to the first embodiment of the present invention
  • FIG. 5 is a flowchart of spent fuel reprocessing method according to a second embodiment of the present invention.
  • FIG. 6 is a schematic sectional elevational view of an apparatus that can be employed for the electrolysis/reduction step of spent fuel reprocessing method according to the second embodiment of the present invention.
  • FIG. 1 is a flowchart of spent fuel reprocessing method according to a first embodiment of the present invention.
  • spent oxide fuel 1 is disassembled and sheared in a disassembly/shear step 2 .
  • all the spent oxide fuel is dissolved by nitric acid in a dissolution step 3 .
  • U exists in a hexavalent state whereas Pu exists in a tetravalent state.
  • FIG. 2 is a schematic sectional elevational view of an apparatus that can be employed for the electrolysis/valence adjustment step 4 of the first embodiment. More specifically, a cathode chamber 27 and an anode chamber 28 are separated from each other by means of a diaphragm 50 in the apparatus. Catholyte 24 is stored in the cathode chamber 27 and a cathode 25 and a reference electrode 30 are dipped in the catholyte 24 . Anolyte 51 is stored in the anode chamber 28 and an anode 26 is dipped in the anolyte 28 .
  • the cathode 25 and the anode 26 are connected to a power source 29 .
  • the cathode 25 and the reference electrode 30 are connected to a potentiometer 31 .
  • the reference electrode 30 may typically be a silver/silver chloride electrode.
  • the cathode chamber 27 is provided with an agitator 52 for agitating the catholyte 24 .
  • Pu can be reduced to trivalent, while maintaining Np as pentavalent by limiting the cathode potential to not higher than ⁇ 100 mV or confining the cathode current density within a range between not less than 20 mA/cm 2 and 40 mA/cm 2 .
  • the U that is partly reduced to tetravalent is employed to reduce Pu from tetravalent to trivalent. Then, U itself is oxidized to become hexavalent.
  • FIG. 3 is a graph showing some of the results obtained by an experiment, which illustrates the correlation between the cathode potential and the current density observed in an electrolysis/valence adjustment step 4 . It is experimentally proved that the cathode potential can be made equal to ⁇ 0.1 V ( ⁇ 100 mV) by making the current density not less than about 20 mA/cm 2 .
  • hexavalent U can be extracted into tributyl phosphate (TBP)—30% dodecane solution by using such a solution in a U extraction step 5 .
  • TBP tributyl phosphate
  • Trivalent ions of Pu and pentavalent ions of Np remain in the aqueous solution with the tetravalent ions of part of U.
  • FIG. 4 is a graph showing some of the results of measurement of the change with time of the current density when the electrolysis potential is held to ⁇ 100 mV relative to the reference electrode, which is a silver/silver salt electrode, in the electrolysis/valence adjustment step 4 and the U extraction step 5 .
  • FIG. 4 shows that the cathode current density is within a range between 20 mA/cm 2 and 40 mA/cm 2 for the cathode potential of ⁇ 100 mV.
  • oxalic acid is added to the aqueous solution that is left after the U extraction step 5 to produce oxalic acid precipitate 7 in an oxalic acid precipitation step 6 .
  • the oxalic acid precipitate 7 contains Pu and minor actinides such as Np, Am and Cm, some of rare earth elements (RE) and some of alkaline-earth metal elements. Of the fission products (FP), alkali metal elements and platinum group elements do not precipitate but are dissolved in the filtrate.
  • U, Pu, minor actinides and rare earth group elements are collected as oxalic acid precipitate 7 in the oxalic acid precipitation step 6 .
  • a chlorination step 8 hydrochloric acid is added to the oxalic acid precipitate 7 and dissolved at not higher than 100° C. and subsequently hydrogen peroxide is added thereto in order to decompose the oxalic acid into water and carbon dioxide.
  • the U, the Pu and the minor actinides in the oxalic acid precipitate 7 are converted into chloride 9 in this chlorination step 8 .
  • a platinum group fission product collection step 14 of collecting platinum group fission products from the oxalic acid precipitate 7 obtained in the oxalic acid precipitation step 6 will be described below by referring to FIGS. 1 and 2 .
  • An apparatus having a structure same as the apparatus shown in FIG. 2 that is employed in the electrolysis/valence adjustment step and the U extraction step may be used in the platinum group fission product collection step 14 .
  • the same apparatus may be used or another apparatus having the same structure or a similar structure may be used.
  • the oxalic acid precipitate 7 contains Pu and minor actinides such as Np, Am and Cm, some of rare earth elements and some of alkaline-earth metal elements.
  • alkali metal elements and platinum group elements are not precipitated by oxalic acid and are dissolved in the filtrate (catholyte) 24 .
  • the filtrate 24 that melts the fission products is put into the cathode chamber 27 and the insoluble cathode 25 is immersed in the filtrate 24 for electrolysis in the platinum group fission product collection step 14 .
  • An applied voltage is observed by measuring the potential difference between the reference electrode 30 and the cathode 25 that are immersed in the cathode chamber 27 for the by means of the potentiometer 31 . It is important to control the potentials so as to deposit Pd, Ru, Rh, Mo and Tc that are platinum group fission products without generating hydrogen.
  • the load of producing nuclear waste glass can be reduced because Pd, Ru, Rh, Mo and Tc that are platinum group fission products do not move into the high level liquid waste. Additionally, the rate of producing high level liquid waste can also be reduced.
  • the hexavalent U that is extracted by TBP—30% dodecane in the U extraction step 5 is washed with nitric acid in a U purification step 11 and subsequently converted into an oxide in a denitration step 12 so as to be collected as high purity UO 2 13 .
  • the high purity UO 2 13 can be used as oxide fuel for light water reactors.
  • FIG. 5 is a flowchart of spent fuel reprocessing method according to a second embodiment of the present invention.
  • FIG. 6 is a schematic sectional elevational view of an apparatus that can be employed for the electrolysis/reduction step of the second embodiment.
  • the sequence down to the oxalic acid precipitation step 6 , where the oxalic acid precipitate 7 containing U, Pu, minor actinides and rare earth elements are collected, is same as that of the first embodiment.
  • This second embodiment has an oxidation/dehydration step 15 and an electrolysis/reduction step 17 instead of the chlorination step 8 , the dehydration step 40 and the molten salt electrolysis step 10 of the first embodiment.
  • the oxalic acid precipitate 7 collected in the oxalic acid precipitation step 6 is heated to remove moisture, while ozone or acidic gas is blown into it, in the oxidation/dehydration step 15 to produce oxides (precipitate oxides) 16 of U, Pu, minor actinides and rare earth elements.
  • the oxides 16 are put into a stainless-steel-made cathode basket 19 and loaded in a molten salt electrolytic cell 22 .
  • the cathode basket 19 containing the oxides 16 of U, Pu, minor actinides and rare earth elements is connected to the cathode and an insoluble anode 20 typically made of platinum or grassy carbon is placed in position.
  • the oxides 16 are put into the stainless-steel-made cathode basket 19 in a mixture of molten salts.
  • the mixture of molten salts is preferably prepared by dissolving an oxide of an alkali metal or an alkaline-earth metal into a molten salt of chloride of an alkali metal or an alkaline-earth metal. More specifically, a mixture of molten salts is preferably prepared by dissolving Li 2 O into a molten salt of LiCl, dissolving MgO into a molten salt of MgCl 2 or dissolving CaO into a molten salt of CaCl 2 .
  • oxygen ions in the oxides 16 are drawn out and the drawn out oxygen ions are removed at the anode as oxygen gas or CO 2 gas. Since alkali metal elements such as Cs, alkaline-earth metal elements such as Sr and rare earth elements such as Ce and Nd that are fission products are dissolved in the molten salts from the cathode basket 19 so that they can be separated from metals of U, Pu and minor actinide metals 18 .
  • the oxides are reduced to become metals at the cathode in a manner as expressed by the formulas shown below.
  • oxygen gas is produced at the anode in a manner as expressed by the formula shown below.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Plasma & Fusion (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Electrolytic Production Of Metals (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
US12/470,226 2008-05-30 2009-05-21 Spent fuel reprocessing method Abandoned US20090294299A1 (en)

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JP2008143431A JP5193687B2 (ja) 2008-05-30 2008-05-30 使用済み燃料再処理方法
JP2008-143431 2008-05-30

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JP (1) JP5193687B2 (ja)
CN (1) CN101593566B (ja)
FR (1) FR2931989A1 (ja)
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FR2971948A1 (fr) * 2011-02-28 2012-08-31 Commissariat Energie Atomique Procede de precipitation d'un ou plusieurs solutes
JP2013122392A (ja) * 2011-12-09 2013-06-20 Toshiba Corp ウランの回収方法
GB2545934A (en) * 2016-01-02 2017-07-05 Richard Scott Ian Single stage reprocessing of spent nuclear fuel

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FR2960690B1 (fr) * 2010-05-27 2012-06-29 Commissariat Energie Atomique Procede de traitement de combustibles nucleaires uses ne necessitant pas d'operation de desextraction reductrice du plutonium
JP5758209B2 (ja) * 2011-06-14 2015-08-05 株式会社東芝 使用済み燃料再処理方法
CN102412002B (zh) * 2011-09-06 2013-10-30 中国原子能科学研究院 N2o4氧化调节钚价态的装置
FR2980468B1 (fr) * 2011-09-26 2014-01-24 Commissariat Energie Atomique Procede de preparation d'un oxyhalogenure et/ou oxyde d'actinide(s) et/ou de lanthanide(s) a partir d'un milieu comprenant au moins un sel fondu
JP5944237B2 (ja) * 2012-06-15 2016-07-05 株式会社東芝 核燃料物質の回収方法
FR2992330B1 (fr) * 2012-06-26 2014-08-08 Commissariat Energie Atomique Procede de separation d'au moins un premier element chimique e1 d'au moins un deuxieme element chimique e2 impliquant l'utilisation d'un milieu comprenant un sel fondu specifique
KR101316925B1 (ko) * 2012-10-08 2013-10-18 한국수력원자력 주식회사 우라늄 폐촉매의 처리방법
RU2561065C1 (ru) * 2014-03-31 2015-08-20 Открытое акционерное общество "Радиевый институт имени В.Г. Хлопина" СПОСОБ ПОЛУЧЕНИЯ СОВМЕСТНОГО РАСТВОРА U И Pu
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US9818496B2 (en) * 2014-08-18 2017-11-14 De Nora Permelec Ltd Method for treating tritium-water-containing raw water
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GB2461370A (en) 2010-01-06
GB2461370B (en) 2010-10-20
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GB0909309D0 (en) 2009-07-15

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