Converging Cooperative Functions into the Nanospace of Covalent Organic Frameworks for Efficient Uranium Extraction from Seawater

The extraction of uranium from seawater is challenging though it offers tremendous potential for the sustainable production of nuclear fuel for the energy sector. Herein, we report a new strategy for efficient extraction of uranium from seawater via converging the cooperative functions of adsorption- photocatalysis into the nanospace of covalent organic frameworks (COFs). Functionalization of the organic linkers in the multicomponent COFs allowed exploration of the relationship between material composition and adsorption-photocatalytic activity for uranium extraction. The presence of amidoxime groups in the COFs offered selective binding sites for uranyl, whilst triazine units and bipyridine-Pd groups acted cooperatively to photo-catalytically reduce adsorbed U(VI) to a U(IV) solid product (UO2) for facile collection. One of our developed COFs, 4-Pd-AO, displayed exceptional performance in sequestering and reducing uranyl from natural seawater, with a high extraction capacity of 4.62 mg U/g per day (average data) under visible light irradiation. Mechanistic studies revealed that 4-Pd-AO not only reduced adsorbed uranyl(VI) to U(IV)O-2, but also generated O-1(2) and superoxide radicals under visible light excitation, thus affording excellent antibacterial and antialgal activities (i.e., anti-biofouling properties) for sustained efficient uranium extraction performance. This pro-of-ofconcept study establishes multicomponent COFs as promising candidates for efficient uranium extraction from seawater. [GRAPHICS] .