Efficient Uranium/Lanthanides Separation from Nuclear Waste via Supramolecular Self‐Assembly of Flexible Molecule: High Capacity, Selectivity, and Fast Recovery

Abstract The accumulation of nuclear waste presents a significant challenge to nuclear energy development. The actinide–lanthanide elements separation from nuclear waste is the key to achieving sustainable development of nuclear energy. Herein, this work presents a selective precipitation method for UO 2 2+ recovery via supramolecular self–assembly using 1,4–bis(imidazol–1–ylmethyl)benzene (BIMB), a flexible, acid–stable and environmentally friendly ligand. BIMB rapidly assembles and forms stable polymers driven by UO 2 2+ , achieving near–complete uranium removal (99.9%) within 10 min, with an adsorption capacity of 714.3 mg g −1 . Compared with the crystallographic data and theoretical calculations results of uranium and lanthanum polymers, the selective self‐assembly behavior of BIMB toward uranium is mainly due to its stronger coordination ability toward UO 2 2+ , and the ligand can form a more stable BIMB@U coordination polymer through stronger hydrogen bonds, more stable coordination structures, and stacking modes. This innovative strategy demonstrates separation factors (SF) of 10 3 –10 4 and a 99.9% uranium recovery from simulated nuclear wastewater, with residual concentrations below US EPA standards (30 ppb). This efficient and straightforward solid–liquid separation approach offers great potential for practical applications in U(VI) remediation and resource recovery.