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Wang et al. report here an ultra-robust imidazolium-decorated covalent organic framework (COF) conjugate fabricated by an ionizing radiation strategy for efficient capture of 99TcO4−, where tunable ReO4− uptake up to 952 mg g−1 can be achieved by simply adjusting the γ-ray dose. The COFs feature high porosity, ultra-robust nanofiber structure, and fast adsorption kinetics, thus emphasizing their advantages in terms of column experiments.

Despite that two-dimensional transition metal carbides and carbonitrides (MXenes) are burgeoning candidates for remediation of environmental pollutants, the construction of robust functionalized MXene nanosheets with a high affinity for target heavy metal ions and radionuclides remains a challenge. Here we report the successful placement of amidoxime chelating groups on Ti3C2Tx MXene surface by diazonium salt grafting. The introduction of amidoxime functional groups significantly enhances the selectivity of Ti3C2Tx nanosheets for uranyl ions and also greatly improves their stability in aqueous solution, enabling efficient, rapid, and recyclable uranium extraction from aqueous solutions containing competitive metal ions. Benefiting from the excellent conductivity of MXenes, the amidoxime functionalized Ti3C2Tx nanosheets show outstanding electrochemical performance such that when loaded on carbon cloth the application of an electric field increases the uranium adsorption capacity from 294 to 626 mg/g, outperforming all organic electrochemical sorption materials reported previously. The present work provides an effective strategy to functionalize MXene nanosheets with fundamental implications for the design of MXene-based selective electrosorption electrode materials.