Mechanistic insights into lanthanide adsorption by 3A/5A molecular sieve in LiCl-KCl molten salt for radioactive waste molten salt regeneration
摘要
The purification of chloride molten salts remains a critical limitation for scaling dry spent-fuel reprocessing. Here we show that 3A and 5A zeolites provide a robust high-temperature route for removing Er(III) from LiCl-KCl eutectics. Adsorption kinetics reveal rapid uptake and near-quantitative removal by 5A, arising from its enlarged pore architecture and accessible ion-exchange sites. Mechanistic analysis indicates a chemisorption-dominated exchange process, while XRD, SEM-EDS and XPS confirm preserved framework integrity and the formation of stable Er-O species under molten-salt conditions. In multi-lanthanide systems, the sieves maintain strong selectivity governed by ionic-radius trends, enabling simultaneous adsorption of several rare-earth elements. By integrating these adsorption behaviours with molten-salt electrochemical refining, this work outlines a cost-efficient strategy for regenerating contaminated salts. The results provide mechanistic insight and a practical pathway toward overcoming a major bottleneck in closing the nuclear fuel cycle, offering a promising direction for next-generation pyroprocessing technologies.