Abstract
The cesium uranates Cs2UO4, Cs2U2O7, Cs4U5O17 and Cs2U4O12 were studied using X-ray Diffraction (XRD), neutron diffraction, X-ray Photoelectron Spectroscopy (XPS) and X-ray Absorption Spectroscopy (XAS) in an attempt to couple the crystallographic structure to the uranium valence state using the local uranium environment. The diffraction spectra were used for Rietveld refinement to determine the atomic positions and interatomic distances. These distances were subsequently used in Bond Valence Sum (BVS) calculations to determine the uranium valences. The XAS spectra give direct information on the local uranium environment regarding the U–O distances and the arrangement of the oxygen atoms around the central uranium. The difference between the monovalent uranates and the multivalent Cs2U4O12 is clearly established in all spectra, as well as in the crystal structures. The different valences present can be assigned to individual uranium lattice sites, but some amount of disorder is required to balance the charges.
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