WO2007135178A1 - Process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide - Google Patents

Process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide Download PDF

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Publication number
WO2007135178A1
WO2007135178A1 PCT/EP2007/055024 EP2007055024W WO2007135178A1 WO 2007135178 A1 WO2007135178 A1 WO 2007135178A1 EP 2007055024 W EP2007055024 W EP 2007055024W WO 2007135178 A1 WO2007135178 A1 WO 2007135178A1
Authority
WO
WIPO (PCT)
Prior art keywords
uranium
plutonium
phase
aqueous
process according
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.)
Ceased
Application number
PCT/EP2007/055024
Other languages
English (en)
French (fr)
Inventor
Pascal Baron
Binh Dinh
Michel Masson
François DRAIN
Jean-Luc Emin
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.)
Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
Orano Demantelement SAS
Original Assignee
Areva NC SA
Commissariat a lEnergie Atomique CEA
Compagnie Generale des Matieres Nucleaires SA
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 NC SA, Commissariat a lEnergie Atomique CEA, Compagnie Generale des Matieres Nucleaires SA filed Critical Areva NC SA
Priority to DE200760003013 priority Critical patent/DE602007003013D1/de
Priority to US12/300,705 priority patent/US20090184298A1/en
Priority to CN2007800188112A priority patent/CN101449338B/zh
Priority to JP2009511522A priority patent/JP5325098B2/ja
Priority to AT07729457T priority patent/ATE447231T1/de
Priority to EP20070729457 priority patent/EP2022061B1/en
Priority to KR1020087028715A priority patent/KR101386696B1/ko
Publication of WO2007135178A1 publication Critical patent/WO2007135178A1/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

Links

Classifications

    • 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
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G43/00—Compounds of uranium
    • C01G43/003—Preparation involving a liquid-liquid extraction, an adsorption or an ion-exchange
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G43/00—Compounds of uranium
    • C01G43/01—Oxides; Hydroxides
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G56/00—Compounds of transuranic elements
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G56/00—Compounds of transuranic elements
    • C01G56/001—Preparation involving a liquid-liquid extraction, an adsorption or an ion-exchange
    • 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
    • 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

  • OXide Fuel nuclear fuels, such as the MIMAS
  • aqueous phase or phases resulting from these coextraction and scrubbing operations which are laden with fission products, are removed from the cycle whereas the solvent phase, which is itself laden with uranium(VI) and with plutonium (IV) , is directed to a zone in which the partition of these two elements is carried out.
  • This partition comprises:
  • the partition further includes a step whose purpose is to remove the uranium from the aqueous nitric phase resulting from the operation of back- extracting the plutonium by means of a solvent phase, of the same composition as that used for coextracting the uranium and plutonium.
  • the first aqueous stream resulting from the first cycle is then subjected to the "second plutonium cycle", the purpose of which is to complete the decontamination of the plutonium from the fission products liable to be still present in trace amounts in this stream. Thereafter, this stream which contains plutonium at a purity level of greater than 99.9%, is directed to a zone where the plutonium is converted into the oxide
  • the neptunium therefore almost quantitatively follows the uranium during all the operations of the first cycle, hence the need to subject the aqueous uranium- laden stream, resulting from the partition, to a complementary cycle suitable for stripping it of the neptunium before it is converted to uranium oxide.
  • the uranium has, after the "second uranium cycle", a purity level of greater than 99.9%. It is also converted to the oxide and stored in this form.
  • Step c) of the process of the invention then preferably comprises, at least:
  • the process according to the invention includes the removal of the neptunium present in the aqueous phase obtained after operation bi) , either during step b) or during step c) .
  • the removal of the neptunium may also be carried out during operation C2) by adding, to the aqueous phase used during this operation, a reducing agent capable of selectively reducing neptunium (VI) to neptunium (V) that is to say without reducing the plutonium or the uranium, and to do so in order to allow the neptunium to pass into the aqueous phase while leaving the plutonium and the uranium in the solvent phase.
  • a reducing agent capable of selectively reducing neptunium (VI) to neptunium (V) that is to say without reducing the plutonium or the uranium, and to do so in order to allow the neptunium to pass into the aqueous phase while leaving the plutonium and the uranium in the solvent phase.
  • the reducing agent capable of reducing plutonium (IV) to plutonium (III) may especially be uranous nitrate or hydroxylammonium nitrate. Preferably either one is used in conjunction with a nitrous acid scavenger, preferably hydrazine.
  • a nitrous acid scavenger preferably hydrazine.
  • the reducing agent capable of reducing neptunium (VI) to neptunium (V) without reducing either the uranium or the plutonium, which is used during operation C2) for removing the neptunium this may especially be a compound of the family of butyraldehydes or hydrazine.
  • the amount of uranium that is introduced into the unit where the "Np scrubbing" takes place is preferably such that the aqueous phase resulting from this operation has a U/Pu mass ratio of around 20/80 to 50/50, and the parameters used to carry out the "Pu/U back-extraction" located downstream of this "Np scrubbing" are preferably adjusted so as to obtain, after this back-extraction, an aqueous phase having a U/Pu mass ratio of around 20/80 to 50/50 and, ideally, of around 20/80 to 30/70. It is desirable to obtain such a ratio in order to minimize the volume of material stored in tanks.
  • the "FP scrubbing" of the purification step is carried out by bringing the solvent phase resulting from this coextraction into contact with an aqueous phase of moderate acidity, for example a 1 to 3M aqueous nitric acid solution, to which has been added a reducing agent capable of reducing neptunium (VI) which is extractable by TBP, to neptunium (V) , which is not extractable by
  • an aqueous phase of moderate acidity for example a 1 to 3M aqueous nitric acid solution
  • This reducing agent is, for example, a butyraldehyde (ButAl) .
  • the neptunium thus passes into the aqueous phase, whereas the plutonium and the uranium remain in the solvent phase.
  • This variant makes it possible, in the case of reprocessing spent nuclear fuels that have cooled for about 10 years or more, to dispense with the operations intended to purify the uranium.
  • the "Pu/U back-extraction" operation of the purification step therefore necessarily includes the addition of a suitable amount of uranium (IV) so as to give the aqueous phase resulting from this operation a U/Pu mass ratio consistent with that which the mixed uranium-plutonium oxide that it is desired to manufacture must have.
  • the process takes place as in the mode of implementation illustrated in Figure 3 except that it does not include the elimination of the neptunium during the "FP scrubbing" of the purification step.
  • Article BN 3650 (07-2000) : The treatise "Genie Nucleaire” - “Techniques de 1' Ingenieur” .

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • Geology (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Extraction Or Liquid Replacement (AREA)
  • Oxygen, Ozone, And Oxides In General (AREA)
PCT/EP2007/055024 2006-05-24 2007-05-23 Process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide Ceased WO2007135178A1 (en)

Priority Applications (7)

Application Number Priority Date Filing Date Title
DE200760003013 DE602007003013D1 (de) 2006-05-24 2007-05-23 Verfahren zur wiederaufbereitung von verbrauchtem kernbrennstoff und zur herstellung eines gemischten uran-plutonium-oxids
US12/300,705 US20090184298A1 (en) 2006-05-24 2007-05-23 Process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide
CN2007800188112A CN101449338B (zh) 2006-05-24 2007-05-23 用于后处理废核燃料及制备混合的铀-钚氧化物的方法
JP2009511522A JP5325098B2 (ja) 2006-05-24 2007-05-23 使用済み核燃料を再処理しウラン・プルトニウム混合酸化物を調製する方法
AT07729457T ATE447231T1 (de) 2006-05-24 2007-05-23 Verfahren zur wiederaufbereitung von verbrauchtem kernbrennstoff und zur herstellung eines gemischten uran-plutonium-oxids
EP20070729457 EP2022061B1 (en) 2006-05-24 2007-05-23 Process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide
KR1020087028715A KR101386696B1 (ko) 2006-05-24 2007-05-23 사용후 핵연료 재처리 및 우라늄-플루토늄 혼합 산화물 제조 방법

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
FR06/04717 2006-05-24
FR0604717A FR2901627B1 (fr) 2006-05-24 2006-05-24 Procede de retraitement d'un combustible nucleaire use et de preparation d'un oxyde mixte d'uranium et de plutonium
US85302406P 2006-10-20 2006-10-20
US60/853,024 2006-10-20

Publications (1)

Publication Number Publication Date
WO2007135178A1 true WO2007135178A1 (en) 2007-11-29

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PCT/EP2007/055024 Ceased WO2007135178A1 (en) 2006-05-24 2007-05-23 Process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide

Country Status (12)

Country Link
US (2) US20090184298A1 (enExample)
EP (1) EP2022061B1 (enExample)
JP (1) JP5325098B2 (enExample)
KR (1) KR101386696B1 (enExample)
CN (1) CN101449338B (enExample)
AT (1) ATE447231T1 (enExample)
DE (1) DE602007003013D1 (enExample)
ES (1) ES2334852T3 (enExample)
FR (1) FR2901627B1 (enExample)
RU (1) RU2431896C2 (enExample)
WO (1) WO2007135178A1 (enExample)
ZA (1) ZA200809415B (enExample)

Cited By (12)

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WO2011000844A1 (fr) 2009-07-02 2011-01-06 Areva Nc Procede ameliore de traitement de combustibles nucleaires uses
WO2011012563A1 (fr) 2009-07-27 2011-02-03 Commissariat A L'energie Atomique Et Aux Energies Alternatives Procede de recuperation selective de l'americium a partir d'une phase aqueuse nitrique
WO2011012579A1 (fr) 2009-07-27 2011-02-03 Commissariat à l'énergie atomique et aux énergies alternatives Augmentation du facteur de separation entre l'americium et le curium et/ou entre des lanthanides dans une operation d'extraction liquide-liquide
WO2011147871A1 (fr) 2010-05-27 2011-12-01 Commissariat à l'Energie Atomique et aux Energies Alternatives Procede de traitement de combustibles nucleaires uses ne necessitant pas d'operation de desextraction reductrice du plutonium
WO2012069573A1 (fr) 2010-11-25 2012-05-31 Commissariat à l'énergie atomique et aux énergies alternatives Procede de separation de l'americium des autres elements metalliques presents dans une phase aqueuse acide ou organique et ses applications
CN102753711A (zh) * 2009-12-22 2012-10-24 原子能与替代能源署 用于从天然铀浓缩物中纯化铀的方法
CN103305702A (zh) * 2013-07-08 2013-09-18 中国原子能科学研究院 一种从Purex流程的2AW+2DW中放废液中回收和纯化镎的工艺
WO2015091791A1 (fr) 2013-12-20 2015-06-25 Commissariat à l'énergie atomique et aux énergies alternatives Procédé de traitement d'un combustible nucléaire usé comprenant une étape de décontamination de l'uranium(vi) en au moins un actinide(iv) par complexation de cet actinide(iv)
RU2561508C1 (ru) * 2014-04-29 2015-08-27 Федеральное государственное унитарное предприятие "Научно-исследовательский технологический институт имени А.П. Александрова" Способ иммобилизации стронций-цезиевой фракции высокоактивных отходов включением в геокерамические матрицы
WO2019115394A1 (en) 2017-12-11 2019-06-20 Orano Cycle Method for preparing a powder comprising particles of triuranium octoxide and particles of plutonium dioxide
US11594344B2 (en) 2017-12-11 2023-02-28 Commissariat à l'énergie atomique et aux énergies alternatives Method for preparing a powder comprising particles of triuranium octoxide and particles of plutonium dioxide
EP4332991A1 (fr) 2022-09-02 2024-03-06 Commissariat à l'énergie atomique et aux énergies alternatives Procédé de désextraction d'uranium(vi) et d'un actinide(iv) d'une solution organique par précipitation oxalique

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FR2947663A1 (fr) * 2009-07-02 2011-01-07 Areva Nc Procede ameliore de traitement de combustibles nucleaires uses
WO2011000844A1 (fr) 2009-07-02 2011-01-06 Areva Nc Procede ameliore de traitement de combustibles nucleaires uses
RU2537952C2 (ru) * 2009-07-02 2015-01-10 Арева Нс Улучшенный способ переработки отработанного ядерного топлива
JP2012531579A (ja) * 2009-07-02 2012-12-10 アレヴァ・エヌセー 使用済み核燃料の改善された処理方法
WO2011012563A1 (fr) 2009-07-27 2011-02-03 Commissariat A L'energie Atomique Et Aux Energies Alternatives Procede de recuperation selective de l'americium a partir d'une phase aqueuse nitrique
WO2011012579A1 (fr) 2009-07-27 2011-02-03 Commissariat à l'énergie atomique et aux énergies alternatives Augmentation du facteur de separation entre l'americium et le curium et/ou entre des lanthanides dans une operation d'extraction liquide-liquide
US8753420B2 (en) 2009-07-27 2014-06-17 Commissariat A L'energie Atomique Et Aux Energies Alternatives Method for selectively recovering americium from a nitric aqueous phase
CN102753711B (zh) * 2009-12-22 2013-08-21 原子能与替代能源署 用于从天然铀浓缩物中纯化铀的方法
CN102753711A (zh) * 2009-12-22 2012-10-24 原子能与替代能源署 用于从天然铀浓缩物中纯化铀的方法
FR2960690A1 (fr) * 2010-05-27 2011-12-02 Commissariat Energie Atomique Procede de traitement de combustibles nucleaires uses ne necessitant pas d'operation de desextraction reductrice du plutonium
WO2011147871A1 (fr) 2010-05-27 2011-12-01 Commissariat à l'Energie Atomique et aux Energies Alternatives Procede de traitement de combustibles nucleaires uses ne necessitant pas d'operation de desextraction reductrice du plutonium
KR101900112B1 (ko) * 2010-05-27 2018-09-18 꼼미사리아 아 레네르지 아토미끄 에뜨 옥스 에너지스 앨터네이티브즈 플루토늄 환원 후-추출 조작이 요구되지 않는 사용된 핵연료 처리방법
US8795610B2 (en) 2010-05-27 2014-08-05 Commissariat A L'energie Atomique Et Aux Energies Alternatives Process for reprocessing spent nuclear fuel not requiring a plutonium-reducing stripping operation
WO2012069573A1 (fr) 2010-11-25 2012-05-31 Commissariat à l'énergie atomique et aux énergies alternatives Procede de separation de l'americium des autres elements metalliques presents dans une phase aqueuse acide ou organique et ses applications
US9051629B2 (en) 2010-11-25 2015-06-09 Commissariat A L'energie Atomique Et Aux Energies Alternatives Process for separating americium from other metallic elements present in an acidic aqueous or organic phase
CN103305702B (zh) * 2013-07-08 2014-12-24 中国原子能科学研究院 一种从Purex流程的2AW+2DW中放废液中回收和纯化镎的工艺
CN103305702A (zh) * 2013-07-08 2013-09-18 中国原子能科学研究院 一种从Purex流程的2AW+2DW中放废液中回收和纯化镎的工艺
WO2015091791A1 (fr) 2013-12-20 2015-06-25 Commissariat à l'énergie atomique et aux énergies alternatives Procédé de traitement d'un combustible nucléaire usé comprenant une étape de décontamination de l'uranium(vi) en au moins un actinide(iv) par complexation de cet actinide(iv)
US10210958B2 (en) 2013-12-20 2019-02-19 Commissariat à l'énergie atomique et aux énergies alternatives Method for processing spent nuclear fuel comprising a step for decontaminating uranium (VI) from at least one actinide (IV) by complexing this actinide (IV)
RU2561508C1 (ru) * 2014-04-29 2015-08-27 Федеральное государственное унитарное предприятие "Научно-исследовательский технологический институт имени А.П. Александрова" Способ иммобилизации стронций-цезиевой фракции высокоактивных отходов включением в геокерамические матрицы
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US11594344B2 (en) 2017-12-11 2023-02-28 Commissariat à l'énergie atomique et aux énergies alternatives Method for preparing a powder comprising particles of triuranium octoxide and particles of plutonium dioxide
EP4332991A1 (fr) 2022-09-02 2024-03-06 Commissariat à l'énergie atomique et aux énergies alternatives Procédé de désextraction d'uranium(vi) et d'un actinide(iv) d'une solution organique par précipitation oxalique
FR3139408A1 (fr) 2022-09-02 2024-03-08 Commissariat A L'energie Atomique Et Aux Energies Alternatives Procédé de désextraction d’uranium(vi) et d’un actinide(iv) d’une solution organique par précipitation oxalique

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US7887767B2 (en) 2011-02-15
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