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Article Abstract
Uranyl-organic coordination polymers (UOCPs) have been demonstrated to exhibit photocatalytic activity, but highly stable UOCPs with excellent photocatalytic efficiency are rare. Herein, we present a series of UOCPs built by a semirigid benzimidazole-derived carboxyl ligand. By rationally designing the rigid and flexible sections of the ligand, we have obtained UO(HBDA)(OH)·HO (), UO(HBDA)(HBDA)(NO)·HO (), and UO(HBDA) () with multiple spatial configurations under different conditions ([HBDA]Cl = 1,3-bis(4-carboxybenzyl)-1,3-dihydro-2-benzo[]imidazol-2-iminium chloride). The structural and photoelectrochemical properties of these UOCPs were systematically investigated, and the relationship between coordination structure and the photocatalytic performance for photooxidation of benzylamine to -benzylenzoimide has been well established. The UOCP-SU-1 with bridged oxygen ligands in the coordination structure exhibits the best visible-light response and chemical conformational stability activity. Importantly, the UOCP-SU-1 can maintain its original crystal structures after 10 cycles of catalysis. This work provides a novel strategy for developing efficient uranyl-based photocatalysts for organic reactions.
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