99TcO4− remediation by a cationic polymeric network

Abstract Direct removal of 99 TcO 4 − from the highly acidic solution of used nuclear fuel is highly beneficial for the recovery of uranium and plutonium and more importantly aids in the elimination of 99 Tc discharge into the environment. However, this task represents a huge challenge given the combined extreme conditions of super acidity, high ionic strength, and strong radiation field. Here we overcome this challenge using a cationic polymeric network with significant TcO 4 − uptake capabilities in four aspects: the fastest sorption kinetics, the highest sorption capacity, the most promising uptake performance from highly acidic solutions, and excellent radiation-resistance and hydrolytic stability among all anion sorbent materials reported. In addition, this material is fully recyclable for multiple sorption/desorption trials, making it extremely attractive for waste partitioning and emergency remediation. The excellent TcO 4 − uptake capability is elucidated by X-ray absorption spectroscopy, solid-state NMR measurement, and density functional theory analysis on anion coordination and bonding.