Abstract
Neodymium−silicon britholites, Ca10-xNdx(PO4)6-x(SiO4)x(OH)2, have been synthesized by the ceramic method. These materials can be used as host matrixes for actinides immobilization and Nd models the actinide. The crystal-chemistry evolution as a function of the Si and Nd content has been studied by combined neutron and X-ray Rietveld refinement. The SiO44- substitution for PO43- does not lead to significant changes in the PO4 tetrahedrons. The Nd3+ cations substitute for Ca2+ and are placed at the Ca(2) sites, getting closer to the hydroxyl sites. The local increase of positive charge around hydroxyls leads to the O2- stabilization in 4e Wyckoff position. Since neutrons are sensitive to the H atoms, the hydroxylation degree has been calculated. Finally, the scattering density Fourier difference maps suggest the presence of HPO42- groups, which partially substitute for PO43- to keep the electric balance of these compounds.
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