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

Regulating the active sites to increase the yield of •OH is a specialized focus for pollutant photodegradation by g-C 3 N 4 -based photocatalysts. Herein, the tertiary N site was first tailored by edge activation to optimize the •OH evolution path. Ethyl alcohol and cyano group comodified g-C 3 N 4 was first fabricated via a facile one-pot thermal copolymerization route to achieve a high yield of •OH. The as-prepared N20–CN exhibited first-class photocatalytic oxidation ability in the degradation of phenol ( k 40 min is 26.3 times higher than that of BCN). Both experimental results and DFT calculations disclose that the tertiary N site with increased electron density via synergy of the two groups realizes not only the oxygen reduction route mediated with •O 2 – but also the in situ conversion of H 2 O 2 between high production and strong reduction, governing the O 2 → •O 2 – → H 2 O 2 → •OH optimal evolution path with a high yield of •OH. This paper provided a theoretical basis for the development of a superactive g-C 3 N 4 -based photocatalyst and optimization of •OH evolution paths via the edge activation strategy for solar-driven photochemical applications.