Abstract
AbstractLnPO4·0.667H2O rhabdophane has been considered as a potential material for the precipitation of actinides from radioactive waste liquid, owing to its outstanding characteristics of high actinide bearing and easy synthesis in acid solutions. However, a comprehensive understanding of the actinide occupation and the precipitation response of rhabdophane to remove actinides has yet to be established. In this study, the effect of ions concentration and pH values on the detailed precipitation reaction of CexNd1‐xPO4·0.667H2O rhabdophane in acid solutions are systematically investigated. Some specific issues such as structural distortion and flexibility, and occupation mechanism are discussed by combining with experiments and density functional theory (DFT) calculation. The results reveal that ions concentration and pH values have a significant impact on the crystallization nucleation step before 12 h. The obtained removal rate of Nd3+is more than 99% in pH 1–5 solutions with the ions concentration of 0.05–0.1 mol/L. Moreover, incorporating Nd in CePO4·0.667H2O rhabdophane will easily result in the lattice distortion inb‐axis. DFT calculation and X‐ray photoelectron spectroscopy (XPS) results reveal that Nd is preferentially incorporated in nonhydrated site to form a weaker binding energy of NdO8polyhedron.
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