Design of dual-defective polymeric carbon nitride with compact interlayer stacking for boosting photocatalytic H2O2 production: Insight of various configurations

Polymeric carbon nitride (PCN) is an environmentally friendly photocatalyst for solar-driven H 2 O 2 production, but the activity of original PCN is still not satisfactory. The main limitation is the sluggish exciton dissociation leading to slow generation and conversion of superoxide radical (•O 2 − ) intermediate. Herein, the PCN with dual defect sites and compact interlayer is rationally designed for H 2 O 2 photosynthesis with an ultrahigh rate of 3930.9 μmol g −1 h −1 and rapid •O 2 − yield rate of 1.92 min −1 . The enhanced activity is attributed to effective exciton dissociation during interlayer and intralayer process. Moreover, nitrogen vacancies change the oxygen adsorption configuration (formation of C − O − O − C bridge mode), thus promoting O 2 adsorption and activation. A well-matched linear relationship was established between the concentration of nitrogen vacancies and •O 2 − /H 2 O 2 production. This work not only provides in-depth insights for the photocatalytic H 2 O 2 generation mechanism, but also offers a new paradigm for designing efficient PCN-based photocatalysts for energy conversion.