Incorporation of uranium to the langbeinite family in Cs2UⅣLn(PO4)3 actinide waste forms
摘要
Langbeinite is proposed as a promising host matrix for radioactive wastes, but no structures incorporating actinides have been reported yet. In this work, a series of single crystals of Cs2UⅣLn(PO4)3 (Ln = Ce – Nd and Sm – Lu), the first reported langbeinite-type structure incorporating actinides (UIV) which crystallizes in the cubic space group P213, have been successfully prepared by optimizing the high-temperature molten salt method. Their 3D frameworks are characterized by a typical langbeinite structure with U/Ln co-occupying six-coordinated octahedra and Cs cations filling closed large-sized cavities. The compounds exhibit high thermal stability up to 1200 °C under N2 and show outstanding leaching resistance, with the leaching rates of U and Nd at 10−8 g·m−2·d−1 and Cs 10−3 g·m−2·d−1. This study highlights the potential of langbeinite-type structures for effectively immobilizing both tetravalent and trivalent actinides as promising waste forms.