Raman micro-spectroscopy of UOX and MOX spent nuclear fuel characterization and oxidation resistance of the high burn-up structure

摘要

Raman micro-spectroscopy was applied to study the structure and oxidation resistance of UO2 (burnup 60 GWd/tHM) and MOX (burnup 47 GWd/tHM) irradiated fuels. The Raman technique, adapted to working under extreme conditions, enabled structural information to be obtained at the cubic micrometer scale in various zones of interest within irradiated fuel (central and zones like the Rim for UOX60, and the plutonium-enriched agglomerates for MOX47 characterized by a high burn-up structure), and the study of their oxidation resistance. As regards the structural information after irradiation, the spectra obtained make up a set of data consistent with the systematic presence of the T-2g band characteristic of the fluorite structure, and of a triplet band located between 500 and 700 cm(-1). The existence of this triplet can be attributed to the presence of defects originating in changes to the fuel chemistry occurring in the reactor (presence of fission products) and to the accumulation of irradiation damage. As concerns the oxidation resistance of the different zones of interest, Raman spectroscopy results confirmed the good stability of the restructured zones (plutonium-enriched agglomerates and Rim) rich in fission products compared to the non-restructured UO2 grains. A greater structural stability was noticed in the case of high plutonium content agglomerates, as this element favors the maintenance of the fluorite structure. (C) 2015 Elsevier B.V. All rights reserved.