US20090184298A1 - 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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US20090184298A1
US20090184298A1 US12/300,705 US30070507A US2009184298A1 US 20090184298 A1 US20090184298 A1 US 20090184298A1 US 30070507 A US30070507 A US 30070507A US 2009184298 A1 US2009184298 A1 US 2009184298A1
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uranium
plutonium
phase
process according
aqueous
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Pascal Baron
Binh Dinh
Michel Masson
Francois Drain
Jean Luc Emin
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Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
Orano Demantelement SAS
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Areva NC SA
Commissariat a lEnergie Atomique CEA
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Publication of US20090184298A1 publication Critical patent/US20090184298A1/en
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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
    • 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

  • the present invention relates to a novel process for reprocessing a spent nuclear fuel, based on uranium oxide or on mixed uranium-plutonium oxide, which makes it possible for the uranium and plutonium to be very effectively decontaminated from other chemical elements contained in this fuel without leaving, at any moment during this process, plutonium without uranium, so as to minimize the risk of misappropriating the plutonium for military purposes.
  • the process of the invention also makes it possible to obtain, at the end of this decontamination, a mixed uranium-plutonium oxide powder that can be used directly in processes for manufacturing MOX (Mixed OXide Fuel) nuclear fuels, such as the MIMAS (MIcronized MASter Blend) process.
  • MOX Mated OXide Fuel
  • MIMAS MIcronized MASter Blend
  • the PUREX process as implemented in modern reprocessing plants such as UP3 and UP2-800 plants on the Areva NC site at La Hague in France, or Rokkasho plant in Japan, schematically comprises three purification cycles: a first cycle, the purpose of which is essentially to decontaminate both the uranium and the plutonium from the fission products and from two minor actinides, namely americium and curium, and also to partition these two elements into two separate streams; and two complementary cycles called the “second plutonium cycle” and “second uranium cycle”, respectively, the purpose of which is to purify the plutonium and the uranium after their partition.
  • a first cycle the purpose of which is essentially to decontaminate both the uranium and the plutonium from the fission products and from two minor actinides, namely americium and curium, and also to partition these two elements into two separate streams
  • two complementary cycles called the “second plutonium cycle” and “second uranium cycle
  • the first cycle starts with an operation which consists in extracting both the uranium and the plutonium, the first being in oxidation state (VI), and the second being in oxidation state (IV), from the aqueous phase in which they are found.
  • This aqueous phase is obtained by dissolving a spent fuel in nitric acid and clarifying the mixture thus obtained. This phase is commonly called the “dissolution liquor”.
  • the coextraction of the uranium and plutonium is carried out by means of a water-immiscible solvent phase that contains an extractant having a high affinity for uranium(VI) and for plutonium(IV), in this case tri-n-butyl phosphate (or TBP) used with a concentration of 30% (v/v) in an organic diluent, in this case a dodecane.
  • TBP tri-n-butyl phosphate
  • 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 (PuO 2 ) and then stored in this form, for the purpose of its subsequent use in the manufacture of MOX nuclear fuel pellets.
  • the second aqueous stream resulting from the first cycle is subjected to the “second uranium cycle”, the purpose of which is to complete the decontamination of the uranium from the fission products, but especially to separate it from the neptunium.
  • neptunium(VI) is reduced by uranous nitrate to neptunium(IV), in which state it can be extracted by TBP, although less than in oxidation state (VI).
  • 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.
  • This method is designed to obtain, after the step of coextracting, the uranium and plutonium in a solvent phase containing, apart from these elements, 0.1 to 10% of the fission products initially present in the dissolution liquor, then to obtain, during the partition step, a plutonium production stream diluted with uranium and containing most of the radioactive fission products present in said solvent phase.
  • This plutonium production stream is then processed by a sol-gel method in order to obtain plutonium-uranium-fission products mixed oxide, which are subsequently used to manufacture fresh nuclear fuels.
  • the inventors were set the objective of providing a process which, like the PUREX process previously described, allows uranium and plutonium to be effectively decontaminated from the other chemical elements present in a spent nuclear fuel, and in particular from the fission products, but which, unlike the PUREX process, at no time leaves plutonium by itself, whether in the solid or liquid state.
  • the inventors were also set the objective that this process should make it possible to obtain a mixed uranium-plutonium oxide that can be directly used for the manufacture of MOX nuclear fuels, whatever the purpose of these fuels: namely fast neutron reactors or light-water reactors.
  • a process for reprocessing a spent nuclear fuel and of preparing a mixed uranium-plutonium oxide which comprises at least:
  • the process of the invention itself proposes to only partially separate the plutonium from the uranium and to keep it, throughout all the consecutive steps of this separation, in the presence of uranium until a mixed uranium-plutonium oxide is obtained.
  • step a) of the process of the invention includes, in addition to a coextraction operation, at least one scrubbing operation carried out on the solvent phase obtained after this coextraction in order to remove from this phase the fission products that were extracted together with the uranium(VI) and the plutonium(IV), this scrubbing operation being performed by bringing said solvent phase into contact with an aqueous nitric phase.
  • step b) of the process of the invention comprises at least:
  • Two aqueous phases are thus obtained, one of which contains plutonium and uranium, while the other contains uranium but does not contain plutonium.
  • Step c) of the process of the invention then preferably comprises, at least:
  • the process of the invention further includes, between these steps, an oxidation operation in order to reoxidize the plutonium(III) present in the aqueous phase obtained after operation b 1 ) to plutonium(IV).
  • This oxidation operation also allows the uranium(IV) also liable to be present in this phase to be reoxidized to uranium(VI) especially if the reducing agent used during operation b 1 ) is uranous nitrate.
  • step b) is carried out in the manner as just described, the aqueous phase obtained after operation b 1 ) inevitably contains neptunium.
  • the process according to the invention includes the removal of the neptunium present in the aqueous phase obtained after operation b 1 ), either during step b) or during step c).
  • This removal of the neptunium may, firstly, be carried out by adding to step b) an operation b 3 ) of re-extracting the neptunium, in oxidation state (IV), from the aqueous phase obtained after operation b 1 ), by bringing this phase into contact with a water-immiscible solvent phase containing at least one extractant in an organic diluent.
  • the invention provides the possibility of adding the uranium either to the aqueous nitric phase subjected to operation b 3 ), or to the aqueous nitric phase subjected to operation c 3 ), or to both, if it is deemed necessary for these phases to be recharged with uranium.
  • the uranium added may be uranium(VI) or uranium(IV).
  • the removal of the neptunium may also be carried out during operation c 2 ) 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 aqueous phase obtained after step c) preferably does not contain more than one ⁇ Ci of fission products per gram of plutonium so as to meet the NF ISO 13463 standard of June 2000 relating to the manufacture of MOX nuclear fuels for light-water reactors.
  • this aqueous phase advantageously has a U/Pu mass ratio ranging from about 20/80 to 50/50.
  • the function of step c) is twofold: namely to purify the plutonium and uranium that are present in the first aqueous phase obtained after step b) with respect to the fission products, on the one hand, and to allow the uranium/plutonium mass ratio to be adjusted on the other hand.
  • Step d) itself is preferably carried out as described in French Patent Application No. 2 870 841, that is to say:
  • the process advantageously also includes a storage step, which consists in storing either the aqueous phase obtained after operation c 3 ) before step d) is carried out, or the mixed uranium-plutonium oxide obtained after step d).
  • This storage step which advantageously corresponds to several months of reprocessing spent nuclear fuels by the process of the invention, for example about 4 to 6 months, makes it possible, on the one hand, to ensure that the workshops responsible for reprocessing spent nuclear fuel are decoupled from those responsible for manufacturing fresh nuclear fuel from the mixed uranium-plutonium oxide obtained after this reprocessing, and on the other hand, to adjust the isotopy of the plutonium to that required by the workshops for manufacturing fresh nuclear fuel.
  • the process of the invention provides, in the case of the aqueous phase obtained after step c 3 ) being stored, for this phase to be subjected:
  • the process of the invention makes it possible to obtain a mixed uranium-plutonium oxide which, depending on whether or not the neptunium present in the aqueous phase after operation b 1 ) has been removed, contains no neptunium or, on the contrary, also contains neptunium.
  • this mixed oxide which is in the form of a powder, can then be used directly for the manufacture of pellets of a mixed nuclear fuel.
  • this mixed oxide preferably has a U/Pu mass ratio of around 50/50 when it does not contain neptunium and a U/Pu/Np mass ratio of around 49/49/2 when it does contain neptunium.
  • the parameters used during the various operations of the process of the invention such as the volume ratios of the solvent phases to the aqueous phases, the number and the duration of the contacting operations between these phases, the acidity of the aqueous phases, etc., and also the amounts of U(VI) or (IV) that can be added during operations b 1 ) and c 3 ), are therefore adjusted accordingly.
  • the extractant for the solvent phases which is used in steps a) and c) and also during the uranium(VI) extraction operation prior to step d) is preferably chosen from extractants that complex the metallic species in oxidation states (IV) and (VI) more strongly than the metallic species in oxidation states (I), (II), (III) and (V), so that uranium(IV), uranium(VI), plutonium(IV), neptunium(IV) and neptunium(VI) are considerably more extractable than plutonium(III) and neptunium(V).
  • This extractant may in particular be a trialkyl phosphate, such as tri-n-butyl phosphate (or TBP), triisobutyl phosphate (TiBP) or a triisoamyl phosphate.
  • TBP tri-n-butyl phosphate
  • TiBP triisobutyl phosphate
  • a triisoamyl phosphate such as tri-n-butyl phosphate (or TBP), triisobutyl phosphate (TiBP) or a triisoamyl phosphate.
  • the organic diluent for this extractant may itself be chosen from various hydrocarbons proposed for liquid-liquid extractions, such as toluene, xylene, t-butylbenzene, triisopropylbenzene, kerosene and linear or branched dodecanes, such as n-dodecane or hydrogenated tetrapropylene (HPT).
  • hydrocarbons proposed for liquid-liquid extractions such as toluene, xylene, t-butylbenzene, triisopropylbenzene, kerosene and linear or branched dodecanes, such as n-dodecane or hydrogenated tetrapropylene (HPT).
  • tri-n-butyl phosphate in a dodecane, and to do so in a volume ratio of around 30/70.
  • the reducing agent capable of reducing plutonium(IV) to plutonium(III), which is used during operations b 1 ) and c 3 ), may especially be uranous nitrate or hydroxylammonium nitrate.
  • 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 c 2 ) for removing the neptunium this may especially be a compound of the family of butyraldehydes or hydrazine.
  • this step comprises:
  • the process of the invention may also include operations of purifying the uranium present in the second aqueous phase obtained after step b), in order to complete its decontamination from the fission products and/or to separate it from the neptunium liable to have followed it in the aqueous phase during operation b 2 ).
  • These operations may be carried out as in any conventional PUREX process (see, for example, the article BN 3 650 (07-2000) of the treatise “GENEe Nucléaire”—“Techniques de l'Ingenieur”).
  • the process according to the invention has many advantages. While being just as effective as the PUREX process in terms of decontamination, unlike the latter, it never allows plutonium to be left without uranium, and thus it minimizes the risk of plutonium being misappropriated for military purposes. It also makes it possible to obtain a mixed uranium-plutonium oxide powder that can be used directly for the manufacture of MOX nuclear fuels for fast neutron reactors or light-water reactors of the second or third generation. Moreover, it is equally applicable to the reprocessing of a spent uranium oxide nuclear fuel as to the reprocessing of a spent mixed uranium-plutonium oxide nuclear fuel.
  • FIG. 1 shows a block diagram of a first embodiment mode of the process of the invention.
  • FIG. 2 shows a block diagram of a first variant of the embodiment mode illustrated in FIG. 1 .
  • FIG. 3 shows a block diagram of a second variant of the embodiment mode illustrated in FIG. 1 .
  • FIG. 4 shows a block diagram of a third variant of the embodiment mode illustrated in FIG. 1 .
  • FIG. 5 shows a block diagram of a second embodiment mode of the process according to the invention.
  • FIG. 1 shows a block diagram of a first embodiment mode of the process of the invention, designed to obtain a mixed uranium-plutonium oxide powder containing no neptunium and able to be used directly in the manufacture of an MOX nuclear fuel, from a dissolution liquor of a spent UO 2 nuclear fuel that has been conventionally prepared, that is to say by dissolving this fuel in nitric acid and clarifying the resulting mixture.
  • Such a dissolution liquor typically contains 200 to 300 g/L of uranium per 2 to 3 g/L of plutonium, i.e. a U/Pu ratio of about 100/1, and has a content of fission products of around 50 to 70 Ci per gram of plutonium.
  • the process of the invention firstly comprises a step designed to separate the uranium and the plutonium from the fission products, the americium and the curium.
  • this separation step comprises:
  • neptunium(IV) is less extractable by TBP than neptunium(VI), it is partially back-extracted during the “Pu/U back-extraction”.
  • the aqueous phase resulting from this operation therefore contains neptunium in addition to plutonium and uranium.
  • the partition step therefore also includes an operation, labelled “Np scrubbing”, which consists in back-extracting the neptunium(IV) present in the aqueous phase resulting from the “Pu/U back-extraction”, by bringing this phase into contact with a solvent phase consisting of about 30% (v/v) TBP in a dodecane, in order to remove from this aqueous phase the neptunium fraction that it contains.
  • Np scrubbing which consists in back-extracting the neptunium(IV) present in the aqueous phase resulting from the “Pu/U back-extraction”, by bringing this phase into contact with a solvent phase consisting of about 30% (v/v) TBP in a dodecane, in order to remove from this aqueous phase the neptunium fraction that it contains.
  • uranium(VI) and neptunium(IV) behave in a relatively similar manner, a fraction of the uranium(VI) present in the aqueous phase resulting from the “U/Pu back-extraction” is re-extracted with the neptunium, which fraction may be relatively large depending on the parameters used to carry out the “Np scrubbing”.
  • uranium may without distinction be uranium(VI) or uranium(IV), may be added in the form of an aqueous nitric solution, it being understood that, if it is uranium(IV), the latter is then stabilized by a nitrous acid scavenger of the hydrazine type.
  • the aqueous phase resulting from the “Np scrubbing” is then subjected to an oxidation operation for bringing the Pu(III) back to oxidation state (IV) and, where appropriate, the U(IV) to oxidation state (VI), before the step of purifying the plutonium and the uranium that it contains is carried out.
  • This oxidation operation may especially be carried out in a conventional manner, that is to say by making said aqueous phase flow, after possibly being diluted with an aqueous nitric phase of high acidity, for example a 12M nitric acid solution, in a stream of nitrogen oxides NO X so as to destroy the nitrous acid scavenger that it contains, thereby making it possible for the nitrous acid to reform and reoxidize the Pu(III) to Pu(IV), the excess nitrous acid then being removed by decomposition to NO and NO 2 and venting of the nitrogen oxides thus formed.
  • an aqueous nitric phase of high acidity for example a 12M nitric acid solution
  • the step of purifying the plutonium and the uranium which follows the partition step and is for the purpose of completing the decontamination of these two elements from the fission products, i.e. so as to obtain in practice an aqueous plutonium-uranium stream preferably having a content of fission products of at most 1 ⁇ Ci per gram of plutonium, comprises:
  • the uranium thus added may be uranium(VI) or uranium(IV), as an aqueous nitric solution containing, in addition, a nitrous acid scavenger if the uranium is uranium(IV).
  • the aqueous phase resulting from the “Pu/U back-extraction”, which is laden with purified plutonium(III) and uranium(IV) or (VI) is itself sent to a unit where, after an oxidation operation for reoxidizing the Pu(III) to Pu(IV) and which is preferably carried out in the same way as the oxidation operation following the “Np scrubbing”, it is subjected to the concentration step in order to increase its plutonium content and its uranium content.
  • the aqueous phase thus concentrated is then stored, for example in tanks with a system of tubes, for a period advantageously corresponding to several months of implementation of the reprocessing process, for example 4 to 6 months, so as to have a stock of purified plutonium and uranium sufficient so that the workshops responsible for manufacturing MOX nuclear fuel are able to work independently of the workshops responsible for reprocessing the spent fuel.
  • This storage also makes it possible to adjust the isotopy of the plutonium to that required for the workshops for manufacturing MOX nuclear fuel.
  • the process of the invention further includes:
  • the aqueous phase resulting from the “U scrubbing” is itself directed to a unit where, after a possible adjustment of its U(IV) content suitable for in this phase a U(Pu) mass ratio consistent with that which the mixed uranium-plutonium oxide that it is desired to prepare must have, the step of coconverting the plutonium and uranium to a mixed oxide is carried out.
  • this coconversion step is preferably carried out according to the process described in FR-A-2 870 841, that is to say by coprecipitation, by oxalic acid or one of its salts or one of its derivatives, of uranium(IV) and plutonium(III) that had been prestabilized by a singly charged cation consisting only of atoms chosen from oxygen, carbon, nitrogen and hydrogen atoms, such as the hydrazinium cation, or by a compound such as a salt, capable of forming such a cation, followed by calcination of the resulting coprecipitate, preferably in an inert or very slightly oxidizing gas, for example a gas containing predominantly argon.
  • a singly charged cation consisting only of atoms chosen from oxygen, carbon, nitrogen and hydrogen atoms, such as the hydrazinium cation, or by a compound such as a salt, capable of forming such a cation, followed by calcination of
  • the mixed uranium-plutonium oxide powder thus obtained can then be used to manufacture MOX nuclear fuel pellets, for example by a MIMAS process, in which case this powder is screened, mixed with uranium oxide and possibly with scrap from the manufacture of pellets in the form of chamotte, and then the resulting mixture undergoes a pelletizing operation followed by a sintering operation.
  • a mixed oxide powder having a U/Pu mass ratio of approximately 50/50.
  • 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.
  • this includes, in addition, operations of purifying the uranium present in the aqueous phase resulting from the “U back-extraction”, which operations are intended to complete its decontamination from the fission products and most particularly to separate it from the neptunium fraction that had followed it during the “Pu/U back-extraction” and the “U back-extraction” of the partition step.
  • These purification operations may be carried out as in any conventional PUREX process and have consequently not been shown in FIG. 1 for the sake of simplifying this figure, nor have they been shown in the following figures.
  • the process of the invention may also include ancillary operations, in particular operations of scrubbing, with pure diluent, the aqueous phases intended to be sent to the vitrification unit and operations of scrubbing and regenerating the spent solvent phases.
  • ancillary operations in particular operations of scrubbing, with pure diluent, the aqueous phases intended to be sent to the vitrification unit and operations of scrubbing and regenerating the spent solvent phases.
  • these operations which are well known in the prior art, have not been shown in FIGS. 1 to 5 for the sake of simplifying these figures.
  • FIG. 2 A block diagram of a first variant of the embodiment mode illustrated in FIG. 1 will now be described with reference to FIG. 2 , in which:
  • 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 TBP, and to do so without reducing either the plutonium or the uranium.
  • 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.
  • the “Pu/U back-extraction” is then carried out in the mode of implementation described above, but by suitably adjusting the parameters of this operation so as to obtain a U/Pu mass ratio of around 20/80 to 50/50 and, ideally, of around 20/80 to 30/70 in the aqueous phase, bearing in mind that the U/Pu mass ratio of the solvent phase resulting from the “FP scrubbing” is likely to be almost the reverse because of the absence of “Np scrubbing”.
  • FIG. 3 shows a block diagram of a second variant of the embodiment mode illustrated in FIG. 1 .
  • This second variant differs from the variant that has just been described in that the reducing agent present in the aqueous phase used during the “Pu/U back-extraction” and “Pu barrage” operations of the partition step is an agent that is capable of reducing plutonium(IV) to plutonium(III) and neptunium(VI) to neptunium(V), respectively, this being the case, for example, of hydroxylammonium nitrate.
  • neptunium(V) Since neptunium(V) is not extractable by TBP, it is therefore completely back-extracted during the “Pu/U back-extraction” and the “Pu barrage” and what are obtained after the partition step are two aqueous phases, one of which, resulting from the “Pu/U back-extraction”contains plutonium, uranium, and neptunium, whereas the other, resulting from the “U back-extraction” contains uranium but does not contain either plutonium or neptunium.
  • 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.
  • FIG. 4 shows schematically yet another variant of the embodiment mode of the process of the invention illustrated in FIG. 1 , which differs from this embodiment mode in that the aqueous phase resulting from the “Pu/U back-extraction” of the purification step is sent directly to a unit where the step of coconverting the plutonium and uranium to a mixed oxide is carried out.
  • 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 decoupling between the workshops responsible for manufacturing MOX nuclear fuel and the workshops responsible for reprocessing spent nuclear fuel is ensured by storing the mixed uranium-plutonium oxide powder obtained after the coconversion step.
  • FIG. 5 illustrates schematically a second embodiment mode of the process of the invention which, unlike the previous ones, is designed to obtain a mixed uranium-plutonium oxide powder, which also contains neptunium, from a dissolution liquor of a spent UO 2 nuclear fuel.
  • the process takes place as in the mode of implementation illustrated in FIG. 3 except that it does not include the elimination of the neptunium during the “FP scrubbing” of the purification step.
  • the neptunium therefore accompanies the plutonium with which it was back-extracted during the “Pu/U back-extraction” throughout all the subsequent steps of the process until a mixed uranium-plutonium-neptunium oxide is obtained.

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US9666315B2 (en) * 2008-08-12 2017-05-30 Kabushiki Kaisha Toshiba Method for reprocessing spent nuclear fuel and centrifugal extractor therefor
US20130202501A1 (en) * 2010-05-27 2013-08-08 Commissariat A L'energie Atomique Et Aux Energies Alternatives Process for reprocessing spent nuclear fuel not requiring a plutonium-reducing stripping operation
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

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US20070290178A1 (en) 2007-12-20
RU2431896C2 (ru) 2011-10-20
ATE447231T1 (de) 2009-11-15
RU2008151145A (ru) 2010-06-27
ES2334852T3 (es) 2010-03-16
ZA200809415B (en) 2009-10-28
FR2901627B1 (fr) 2009-05-01
KR101386696B1 (ko) 2014-04-18
US7887767B2 (en) 2011-02-15
WO2007135178A1 (en) 2007-11-29
KR20090010217A (ko) 2009-01-29
JP2009537838A (ja) 2009-10-29
FR2901627A1 (fr) 2007-11-30
EP2022061A1 (en) 2009-02-11
JP5325098B2 (ja) 2013-10-23
EP2022061B1 (en) 2009-10-28
CN101449338A (zh) 2009-06-03
DE602007003013D1 (de) 2009-12-10

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