Abstract
Despite the pivotal role ofmolecular oxygen (O2) activationin artificial photosynthesis, the activation efficiency is often restricted by sluggish exciton dissociation and charge transfer kinetics within polymer photocatalysts. Herein, weproposetwo tetrathiafulvalene (TTF)-based imine-linked covalent organic frameworks (COFs) withtailored donor-acceptor (D-A) structures, TTF-PDI-COF and TTF-TFPP-COF,to promoteO2activation.Because ofenhanced electron push-pull interactions that facilitated charge separation and transfer behavior, TTF-PDI-COF exhibitedsuperiorphotocatalytic activity in electron-induced O2activationreactionsoverTTF-TFPP-COF under visible light irradiation, includingthe photosynthesis of (E)-3-amino-2-thiocyano-α,β-unsaturated compoundsandH2O2.These findings highlight the significant potential of therational design of COFs with D-A configurationsas suitable candidates for advancedphotocatalytic applications.
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