Incorporation of uranium to the langbeinite family in Cs2UⅣLn(PO4)3 actinide waste forms
Yu Wang1,2,3, Lanxin Li1, Tao Bo1,2
1Zhejiang Key Laboratory of Data-Driven High-Safety Energy Materials and Applications, Ningbo Key Laboratory of Special Energy Materials and Chemistry, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, China.
Abstract:
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.
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