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Impact of platinum group metals (Ru, Pd, Rh) on the dissolution of UO2

Authors :
Solène Bertolotto
Laurent Claparede
Renaud Podor
T. Cordara
Claire Lavalette
Nicolas Dacheux
Stéphanie Szenknect
Adel Mesbah
Interfaces de Matériaux en Evolution (LIME)
Institut de Chimie Séparative de Marcoule (ICSM - UMR 5257)
Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)
Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)
Northwestern University [Evanston]
Etude de la Matière en Mode Environnemental (L2ME)
Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)
Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)
Source :
Journal of Nuclear Materials, Journal of Nuclear Materials, Elsevier, 2020, 528, pp.151836. ⟨10.1016/j.jnucmat.2019.151836⟩, Journal of Nuclear Materials, 2020, 528, pp.151836. ⟨10.1016/j.jnucmat.2019.151836⟩
Publication Year :
2020
Publisher :
Elsevier BV, 2020.

Abstract

International audience; The effect of metallic particles containing Platinum Group Metal (PGM) elements on the dissolution of sintered UO2 samples was examined through the development of multiparametric dissolution tests on sintered UO2 and UO2 + 3 mol.% PGM samples. This effect was found to be more important for CHNO3 < 1 mol L−1 whereas it was lowered for higher nitric acid concentrations due to the preponderant oxidation of U(IV) by nitrate ions. Increase of the normalised dissolution rate of the ceramics was associated to the presence of PGM elements along with the decrease of the duration of the induction period (the stronger effect being observed for ruthenium). Simultaneously, the decrease of the apparent activation energy associated to the reaction of dissolution supported the existence of catalytic effect. This latter was connected to redox reaction between the metallic particles and nitrate ions either in solution or at the PGM/UO2/solution interface. The involved reactions induced the formation of nitrogen species close to the PGM bearing particles. Among them, nitrous acid played an important role due to its strong oxidative power regarding to U(IV). Additionally, no synergistic effect was evidenced when mixing the three PGM elements.

Details

ISSN :
00223115
Volume :
528
Database :
OpenAIRE
Journal :
Journal of Nuclear Materials
Accession number :
edsair.doi.dedup.....74fbbd50e947080a8ed503e5e1d8feeb