“…Currently, the further development of POMOF catalysts requires a deep understanding of their catalytic mechanisms, which is important for guiding the structural design and functional optimization of POMOF catalysts. [42][43][44] Herein, for achieving a highly efficient catalyst for the oxidation of benzylic C-H bonds and a suitable model for mechanistic studies, we constructed a novel polyoxovanadatebased MOF, [Cu I 2 Cu II (bix) 2 ]{V 4 O 12 } (1, bix ¼ 1,4-bis(imidazole-1-ylmethyl)benzene). The structure of 1 contains three possible active centers in close proximity, V V in the highly oxidized state in the unique U-type {V 4 } cluster, Cu I with redox ability and Cu II with coordination unsaturation.…”