A selective solubility-driven separation of used nuclear fuel

Used nuclear fuel (UNF) is a chemically diverse and radiologically hazardous material, though rather than classify it as a waste product, reprocessing seeks to extract one or more of its rare and valuable components. Beyond recoverable fuel materials, UNF contains radioisotopes necessary for theragnostic medicine, radio thermal generators, and stable rare-earth and noble metal elements. An actinide separation scheme is presented herein which deviates substantially from the solvent-extraction approaches most commonly employed. Our method instead opts for low temperature fluorination followed by selective dissolution and antisolvent recrystallization of tetraammonium uranium octafluoride. A variety of applicable antisolvents and a broad workable temperature range demonstrate the potential for process tunability towards the recovery of various UNF components. The exploratory separation scheme is demonstrated to remove 91% of fission-product generated activity from UNF in a single pass. These initial results demonstrate a promising advance toward multi-purpose, proliferation resistant nuclear fuel reprocessing. Reprocessing used nuclear fuel (UNF) can recover valuable components, including radioisotopes for medicine and energy applications. Here, the authors introduce an actinide separation method using low-temperature fluorination, selective dissolution, and antisolvent-recrystallization achieving 91% removal of fission-product generated activity from UNF in a single pass.