Redox‐Active Two‐Dimensional Covalent Organic Frameworks (COFs) for Selective Reductive Separation of Valence‐Variable, Redox‐Sensitive and Long‐Lived Radionuclides

We report the first example of 2D covalent organic framework nanosheets (Redox-COF1) for the selective reduction and in situ loading of valence-variable, redox-sensitive and long-lived radionuclides (abbreviated as VRL nuclides). Compared with sorbents based on chemical adsorption and physical adsorption, the redox adsorption mechanism of Redox-COF1 can effectively reduce the impact of functional group protonation under the usual high-acidity conditions in chemisorption, and raise the adsorption efficiency from the monotonous capture by pores in physisorption. The adsorption selectivity for UO22+ reaches up to unprecedented ca. 97 % at pH 3, more than for any analogous adsorbing material.