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Structural Investigation of (U 0.7 Pu 0.3 )O 2-x Mixed Oxides

Abstract : Uranium-plutonium mixed oxide containing 30 per cent of plutonium is a candidate fuel for several fast neutron and accelerator driven reactor systems. In this work, a detailed structural investigation on sol-gel synthesized stoichiometric U0.7Pu0.3O2.00 and substoichiometric U0.7Pu0.3O2-x, using X-ray diffraction (XRD), oxygen 17 magic angle spinning nuclear magnetic resonance ((17)O MAS NMR) and X-ray absorption spectroscopy is described. As observed by XRD, the stoichiometric U0.7Pu0.3O2.00 is monophasic with a lattice parameter in good agreement with Vegard's law, while the substoichiometric U0.7Pu0.3O2-x material is biphasic. Solid solution ideality in terms of a random distribution of metal atoms is proven for U0.7Pu0.3O2.00 with (17)O MAS NMR. X-ray absorption near-edge structure (XANES) spectroscopy shows the presence of plutonium(III) in U0.7Pu0.3O2-x. Extended X-ray absorption fine-structure (EXAFS) spectroscopy indicates a similar local structure around both cations, and comparison with XRD indicates a close similarity between uranium and plutonium local structures and the long-range ordering.
Keywords : XRD
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https://hal-cea.archives-ouvertes.fr/cea-02386006
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Submitted on : Friday, November 29, 2019 - 10:30:26 AM
Last modification on : Tuesday, April 28, 2020 - 11:28:14 AM

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J.F. Vigier, P.M. Martin, D. Prieur, Ac. Scheinost, J. Somers. Structural Investigation of (U 0.7 Pu 0.3 )O 2-x Mixed Oxides. Inorganic Chemistry, American Chemical Society, 2015, 54 (11), pp.5358-5365. ⟨10.1021/acs.inorgchem.5b00392⟩. ⟨cea-02386006⟩

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