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Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis

Thomas Dumas 1 Matthieu Virot 2 Denis Menut 3 Christelle Tamain 1 Cyril Micheau 2 Sandrine Dourdain 4 Olivier Diat 5 
1 LILA - Laboratory of Interactions Ligand-Actinide
DMRC - Département de recherche sur les procédés pour la mine et le recyclage du combustible : DEN/DMRC
2 LSFC - Sonochimie dans les Fluides Complexes
ICSM - UMR 5257 - Institut de Chimie Séparative de Marcoule
4 LTSM - Tri ionique par les Systèmes Moléculaires auto-assemblés
ICSM - UMR 5257 - Institut de Chimie Séparative de Marcoule
5 L2IA - Ions aux Interfaces Actives
ICSM - UMR 5257 - Institut de Chimie Séparative de Marcoule
Abstract : The size and shape of a water-soluble hexanuclear plutonium cluster were probed by combining synchrotron small-angle X-ray scattering (SAXS) and extended X-ray absorption fine structure (EXAFS). A specific setup coupling both techniques and dedicated to radioactive samples on the MARS beamline endstation at Synchrotron SOLEIL is described. The plutonium hexanuclear cores are well stabilized by the 1,4,7,10 tetraazacyclododecane-1,4,7,10-tetraacetic acid ligands and this allows a good evaluation of the setup to probe the very small plutonium core. The results show that, in spite of the constrained conditions required to avoid any risk of sample dispersion, the flux and the sample environment are optimized to obtain a very good signal-to-noise ratio, allowing the detection of small plutonium aggregates in an aqueous phase. The structure of the well defined hexanuclear cluster has been confirmed by EXAFS measurements in solution and correlated with SAXS data processing and modelling. An iterative comparison of classical fit models (Guinier or sphere form factor) with the experimental results allowed a better interpretation of the SAXS signal that will be relevant for future work under environmentally relevant conditions.
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https://hal-cea.archives-ouvertes.fr/cea-03630418
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Submitted on : Tuesday, July 5, 2022 - 3:39:32 PM
Last modification on : Friday, August 5, 2022 - 10:56:49 AM

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Thomas Dumas, Matthieu Virot, Denis Menut, Christelle Tamain, Cyril Micheau, et al.. Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis. Journal of Synchrotron Radiation, International Union of Crystallography, 2022, 29 (1), pp.30. ⟨10.1107/S1600577521012005⟩. ⟨cea-03630418⟩

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