Boosting excitons dissociation in defective-rich graphitic carbon nitride for efficient hydrogen peroxide photosynthesis and on-site environmental governance

Abstract

Solar-driven hydrogen peroxide (H2O2) production offers a sustainable strategy to address the ever-growing demand of eco-friendly oxidant and clean fuel, while its efficiency highly relies on the generation of desired reactive oxygen species (ROSs). Herein, we demonstrate that introducing boron-nitrogen vacancy (B-NV) associates in g-C3N4 enables to weaken the robust excitonic effect and promote bound excitons spontaneously dissociating into free charge carriers under ambient conditions. Specifically, the doped B atoms introduced a donor state below the conduction band of g-C3N4, which disturbs charge distribution around heptazine rings and further destabilizes excitons. The concomitant NV, serving as an accepter state locating above the valence band, cooperates with the doped B atoms to form B-NV associates that simultaneously downshifts the conduction band and valence band of g-C3N4. Distinct from the counterpart preferring to activate O2 into 1O2 via an energy-transfer-involved pathway, g-C3N4 featuring with B-NV associates displayed a superior photoactivity of visible-light-driven two-electron oxygen reduction reaction for H2O2 production with a yield of 182 μmol h−1 and selectivity of 100%. The produced H2O2 could effectively degrade organic contaminants and kill typical bacteria. This study highlights the importance of ROSs generation in two-dimensional photocatalysts for sustainable solar-to-chemical conversion and on site environmential governance.