Impact of the cation distribution homogeneity on the americium oxidation state in the U0.54Pu0.45Am0.01O2−x mixed oxide

Autor: Anne-Charlotte Robisson, Renaud C. Belin, Fiqiri Hodaj, Philippe Martin, Andreas C. Scheinost, Romain Vauchy, Laurence Aufore
Přispěvatelé: Science et Ingénierie des Matériaux et Procédés (SIMaP), Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Chimie du CNRS (INC)-Institut National Polytechnique de Grenoble (INPG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)
Jazyk: angličtina
Rok vydání: 2015
Předmět:
Zdroj: Journal of Nuclear Materials
Journal of Nuclear Materials, Elsevier, 2015, 456, pp.115-119. ⟨10.1016/j.jnucmat.2014.09.014⟩
ISSN: 0022-3115
DOI: 10.1016/j.jnucmat.2014.09.014⟩
Popis: The impact of the cation distribution homogeneity of the U 0.54 Pu 0.45 Am 0.01 O 2 − x mixed oxide on the americium oxidation state was studied by coupling X-ray diffraction (XRD), electron probe micro analysis (EPMA) and X-ray absorption spectroscopy (XAS). Oxygen-hypostoichiometric Am-bearing uranium–plutonium mixed oxide pellets were fabricated by two different co-milling based processes in order to obtain different cation distribution homogeneities. The americium was generated from β − decay of 241 Pu. The XRD analysis of the obtained compounds did not reveal any structural difference between the samples. EPMA, however, revealed a high homogeneity in the cation distribution for one sample, and substantial heterogeneity of the U–Pu (so Am) distribution for the other. The difference in cation distribution was linked to a difference in Am chemistry as investigated by XAS, with Am being present at mixed +III/+IV oxidation state in the heterogeneous compound, whereas only Am(IV) was observed in the homogeneous compound. Previously reported discrepancies on Am oxidation states can hence be explained by cation distribution homogeneity effects.
Databáze: OpenAIRE