Abstract
Direct removal of 99TcO4− 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 99Tc 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 TcO4− 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 TcO4− uptake capability is elucidated by X-ray absorption spectroscopy, solid-state NMR measurement, and density functional theory analysis on anion coordination and bonding.
Highlights
Direct removal of 99TcO4− 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 99Tc discharge into the environment
SCU-cationic polymeric network (CPN)-1-Br was derived from the quaternization reaction between 1,1,2,2-tetrakis(4-(imidazolyl-4-yl) phenyl)ethene (TIPE) and 1,4-bis(bromomethyl)benzene (BBB) (Fig. 1a)
PXRD measurement confirms the amorphous nature of this material (Supplementary Fig. 1), which is similar to many other CPN materials reported[41,42]
Summary
Direct removal of 99TcO4− 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 99Tc discharge into the environment. They are endowed with a series of excellent features similar with MOFs including predictable reticular synthesis and structure type, controllable pore size/shape/charge, and facile functionalization tailored for trapping targeted environmental pollutants[31,32,33,34,35,36,37] These materials exhibit superior hydrolytic stability even in highly acidic/basic solutions[38,39,40], a clear advantage not possessed by the majority of MOFs. In addition, polymeric network equipped with relatively large conjugated fragments in the structure may show enhanced radiation-resistance compared to traditional polymeric anion-exchange resins because they can effectively stabilize radiation-induced radical intermediates, another merit critical for nuclear-related applications, especially used fuel reprocessing.
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