99TcO4− remediation by a cationic polymeric network

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. Direct removal of 99TcO4− from highly radioactive and acidic nuclear waste solutions is beneficial for uranium and plutonium recovery and radioactive pollution control but this represents a huge challenge. Here the authors show a cationic polymeric network with high 99TcO4− sorption capability and stability.

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Identifiers

DOI

10.1038/s41467-018-05380-5

Journal

Nature Communications

Year

2018