The application of HEXS and HERFD XANES for accurate structural characterization of actinide nanomaterials: application to ThO2.
2020
Structural characterization of actinide nanoparticles (NPs) is of primary importance and hard to achieve, especially for non-homogeneous samples with NPs below 3 nm. By combining High Energy X-ray Scattering (HEXS) and High-Energy-Resolution Fluorescence Detected X-ray Near-Edge Structure (HERFD XANES), we characterized for the first time both short- and medium-range order of ThO 2 NPs obtained by chemical precipitation. With this methodology, a novel insight into the structure of NPs at different steps of their formation process is achieved. The Pair Distribution Function (PDF) reveals a high concentration of ThO 2 small units similar to Th hexamer clusters mixed with 1 nm ThO 2 NPs in the initial steps of formation. Drying the precipitates at ⁓150 °C promotes recrystallization of the smallest units into more thermodynamically stable ThO 2 NPs. HERFD XANES at Th M 4 edge, a direct probe of the f states, shows variations that we correlate to the break of the local symmetry around Th atoms, which most likely concerns surface atoms. Together, HEXS and HERFD are a powerful methodology to investigate actinide NPs and their formation mechanism.
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