This study designs benzotrithiophene-based covalent organic frameworks with spatially separated redox centers for the photocatalytic production of hydrogen peroxide. The triazine-containing framework demonstrates high selectivity for H2O2 photogeneration, with a yield rate of 2111μMh(-1) and a solar-to-chemical conversion efficiency of 0.296%.
Constructing photocatalytically active and stable covalent organic frameworks containing both oxidative and reductive reaction centers remain a challenge. In this study, benzotrithiophene-based covalent organic frameworks with spatially separated redox centers are rationally designed for the photocatalytic production of hydrogen peroxide from water and oxygen without sacrificial agents. The triazine-containing framework demonstrates high selectivity for H2O2 photogeneration, with a yield rate of 2111 mu Mh(-1) (21.11 mu mol h(-1) and 1407 mu mol g(-1) h(-1)) and a solar-to-chemical conversion efficiency of 0.296%. Codirectional charge transfer and large energetic differences between linkages and linkers are verified in the double donor-acceptor structures of periodic frameworks. The active sites are mainly concentrated on the electron-acceptor fragments near the imine bond, which regulate the electron distribution of adjacent carbon atoms to optimally reduce the Gibbs free energy of O-2* and OOH* intermediates during the formation of H2O2.
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