Regulation of the Tertiary N Site by Edge Activation with an Optimized Evolution Path of the Hydroxyl Radical for Photocatalytic Oxidation

Regulatingthe active sites to increase the yield of center dot OHis a specialized focus for pollutant photodegradation by g-C3N4-based photocatalysts. Herein, the tertiary N site wasfirst tailored by edge activation to optimize the center dot OH evolutionpath. Ethyl alcohol and cyano group comodified g-C3N4 was first fabricated via a facile one-pot thermal copolymerizationroute to achieve a high yield of center dot OH. The as-prepared N20-CNexhibited first-class photocatalytic oxidation ability in the degradationof phenol (k (40 min) is 26.3 timeshigher than that of BCN). Both experimental results and DFT calculationsdisclose that the tertiary N site with increased electron densityvia synergy of the two groups realizes not only the oxygen reductionroute mediated with center dot O-2 (-) but alsothe in situ conversion of H2O2 between highproduction and strong reduction, governing the O-2 ->center dot O-2 (-) -> H2O2 -> center dot OH optimal evolution path with a high yieldof center dot OH. This paper provided a theoretical basis for the developmentof a superactive g-C3N4-based photocatalystand optimization of center dot OH evolution paths via the edge activationstrategy for solar-driven photochemical applications.