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Abstract:Solar-driven CO2 reduction reaction with water to value-added chemicals is a promising way to achieve carbon neutrality. Managing the surface microenvironment and electron configuration of catalysts significantly influences photocatalytic efficiency. Herein, fluorinated graphitic carbon nitride (FGCN) with a porous hierarchical structure was prepared by the supramolecular self-assembly method using tetrafluoroterephthalic acid as an introduced monomer. Experimental results and theoretical calculations reveal that fluorine can not only improve the surface microenvironment of carbon nitride and enhance the adsorption of CO2 molecules, but also regulate the local electron structure of catalysts and improve the photogenerated carrier separation efficiency. FGCN demonstrates superior CO2 photoreduction ability in the pure water system, producing CO at a rate of 1.01 mu mol g- 1 h- 1, which is approximately 3.6 times greater than that of the pristine bulk carbon nitride (BCN) sample. This work provides a facile strategy for doping heteroatoms into metal-free carbon nitride catalysts for improving CO2 photoreduction efficiency in water.

Volume:1017

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Translation or Not:no