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Article Abstract
By modifying the coordination environment of single-Fe-atom active site, effective regulation of the photocatalytic oxygen reduction pathway can be achieved to attain high activity for photocatalytic oxidation of CH to CHOH in an aqueous solution. A comprehensive investigation is conducted to study the impact of different coordination numbers of single Fe atoms on photocatalytic CH oxidation reaction over carbon nitride. Among which, Fe/CN with a Fe-N3 coordination exhibit an exceptional photocatalytic performance in CH oxidation, reaching a remarkable methanol yield of 928.27 µmol g , much higher than Fe/CN and Fe/CN (308.47 and 473.26 µmol g , respectively). Based on a collection of in situ characterizations and time-dependent density functional theory calculations, it is determined that Fe/CN with an optimal coordination number possesses the optimized electronic configuration that enables three-electron oxygen reduction to generate hydroxyl radicals for photocatalytic conversion of CH to CHOH.
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