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Royal Society of Chemistry, Dalton Transactions, 14(44), p. 6391-6399

DOI: 10.1039/c4dt03515a

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In situ characterization of uranium and americium oxide solid solution formation for CRMP process: First combination of in situ XRD and XANES measurements

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Abstract

Transmutation of americium in heterogeneous mode through the use of U1-xAmxO2±δ ceramic pellets, also known as Americium Bearing Blankets (AmBB), has become a major research axis. Nevertheless, in order to consider future large-scale deployment, processes involved in the AmBB fabrication have to minimize fine particles dissemination, due to americium presence, which considerably increases the risk of contamination. New synthesis routes avoiding the use of pulverulent precursors are thus currently under development, such as the Calcined Resin Microsphere Pelletization (CRMP) process. It is based on the use of weak-acid resin (WAR) microspheres as precursors, loaded with actinide cations. After two specific calcinations under control atmospheres, resin microspheres are converted into oxide microspheres composed of a monophasic U1-xAmxO2±δ phase. Understanding the different mechanisms implied during thermal conversion, leading to the release of organic matter and the formation of a solid solution, appeared essential. By combining in-situ technics such as XRD and XAS, it has become possible to identify the key temperatures for oxide formation, and the corresponding oxidation states taken by uranium and americium during mineralization. This paper thus presents the first results on the mineralization of (U,Am) loaded resin microspheres into a solid solution, through in-situ XAS analysis correlated with HT-XRD.