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Article Abstract
High-efficiency production of triplet states in covalent organic framework photocatalysts is crucial for high-selectivity oxygen (O) reduction to hydrogen peroxide (HO). Herein, fluorine and partial fluorine atoms are incorporated into an olefin-linked triazine covalent organic framework (F-ol-COF and HF-ol-COF), in which the adjacent fluorine (F) atoms-olefinic bond forms p-π conjugation that induces spin-polarization under irradiation, thus expediting triplet excitons for activating O to singlet oxygen (O) and contributing to a high HO selectivity (91%). Additionally, the feasibility of coupling HO production with the valorization of 5-hydroxymethylfurfural (HMF) is exhibited. The F-ol-COF demonstrates a highly stable HO yield rate of 12558 µmol g h with the HMF-to-functionalized furan conversion yield of 95%, much higher than the partially fluorinated COF (HF-ol-COF) and the non-fluorinated COF (H-ol-COF). Mechanistic studies reveal that F-incorporation promotes charge separation, intensifies the Lewis acidity of the carbon atoms on the olefinic bond as active sites for O adsorption, and provides highly concentrated holes at the triazine unit for HMF oxidation upgrading. This study suggests the attractive potential of rational design of porous-crystalline photocatalysts for high-efficiency photocatalytic O reduction to HO and biomass upgrading.
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