First principles study of volatile fission products trapping properties and chromium doping in actinide oxides
Gascoin, Mathieu; Klosek, Vincent; Freyss, Michel; Njifon, Ibrahim Cheik
Nufuel 2023: Book of abstracts2023
Nufuel 2023: Book of abstracts2023
AbstractAbstract
[en] UO2 and (U,Pu)O2 are the most used fuels in the current nuclear reactor fleet. Under irradiation in a reactor, new chemical elements are created in these materials by the fission of uranium and plutonium nuclei. Some of these fission products, especially iodine, caesium and tellurium may chemically react with one another to form compounds that are potentially corrosive for the cladding. One way to avoid the cladding corrosion consists of preventing the formation and migration of such corrosive species within the fuel. To that end, the determination of the most stable chemical forms of iodine, caesium and tellurium in the fuel as well as the trapping and diffusion mechanisms of these elements in UO2 and (U,Pu)O2 is of first interest. The gain of Cr-doped UO2 fuel on the fission gas retention has already been demonstrated experimentally. However, no data are yet available on the release of corrosive fission products in Cr-doped UO2. With a view to simulating the behaviour of these species within Cr-doped UO2, one has to prior identify the most favourable oxidation state and location site of Cr in UO2, which is a much debated topic in the literature. We perform electronic structure calculations, using the Hubbard-corrected density functional theory (DFT+U) to evaluate the preferred trapping site of I, I2, Cs and Te in UO2 and (U,Pu)O2 crystals, as well as the preferred oxidation state and location of Cr in UO2. We first determine the stability of I, I2, Cs, Te and Cr in various point defects and then compute their XANES spectra in each considered site, using the FDMNES code and the DFT+U atomic configurations. The comparison of the computed spectra with the experimental ones contributes to the identification of the chemical forms and the trapping sites of iodine, caesium, tellurium and chromium in the actinide oxides. The use of a Hubbard term (GGA+U) allows us to take into account the strong correlations of the actinide 5f electrons. To avoid the metastable states inherent to this method, we use the occupation matrix control (OMC) procedure, which also allows us to control the valences of each species in the simulation. This particular point makes our approach reliable with respect to the determination of fission products incorporation energies in the various studied defects. (authors)
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CEA, IRESNE, Direction des Energies (France); Joint Research Centre of the European Commission - JRC, Bruxelles (Belgium); Romanian Institute for Nuclear Research - RATEN, Arges County (Romania); 71 p; 2023; p. 28; Nufuel 2023: Research into nuclear fuel in Europe; Marseille (France); 7-9 Nov 2023; 4 refs.; Available from the INIS Liaison Officer for France, see the INIS website for current contact and E-mail addresses
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Miscellaneous
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Conference
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ACTINIDE COMPOUNDS, ALKALI METALS, CALCULATION METHODS, CHALCOGENIDES, DEPOSITION, ELEMENTS, ENERGY SOURCES, FUELS, HALOGENS, ISOTOPES, MATERIALS, METALS, NONMETALS, NUCLEAR REACTIONS, OXIDES, OXYGEN COMPOUNDS, RADIOACTIVE MATERIALS, REACTOR MATERIALS, SEMIMETALS, SURFACE COATING, TRANSITION ELEMENTS, URANIUM COMPOUNDS, URANIUM OXIDES, VARIATIONAL METHODS
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