Defect Engineering Enhancing Piezoelectric Catalytic Activity of Covalent Organic Framework Matrix Composites for Uranium Removal

Abstract Piezoelectric catalysis is an emerging green strategy, but the existing piezoelectric heterostructures are not sufficient in performance for catalytic reduction of low‐reduction potential uranium under harsh conditions. This study innovatively employs a defect heterogeneous engineering strategy, wherein covalent organic frameworks (COFs) are grown in situ on the surface of zinc oxide (ZnO) via Schiff base reactions, and defects are introduced into the COF shell layer via imine exchange reactions to construct D‐COF@ZnO for piezoelectric catalytic uranium removal. The comprehensive study shows that defect heterogeneous engineering increases the asymmetry induced polarization of the material to promote charge redistribution, and thus significantly improves the activity of piezoelectric catalysis. In addition, defect engineering optimizes the nanosize of D‐COF@ZnO to expose a richer array of active sites, resulting in ultra‐fast U(VI) removal kinetics and ultra‐high removal capacity. In the actual nuclear wastewater settings, D‐COF@ZnO demonstrates outstanding selective removal efficacy for uranium, manifesting its considerable application potential and efficiency superiority. This strategy holds profound implications for facilitating the application of piezoelectric catalytic technology in environmental protection domains such as uranium removal, manifesting its considerable potential and value.