Modulation of Lewis acidic-basic sites for efficient photocatalytic H2O2 production over potassium intercalated tri-s-triazine materials

Abstract

Photocatalytic H2O2 production (PHOP) on graphitic carbon nitride (GCN) at neutral pHs is limited by the sluggish oxidation of sacrificial alcohols and insufficient protons. In our work, the PHOP over a series of K intercalated triazine (KTCN) or tri-s-triazine units (KTTCN) reached 11–32 folds of GCN in the presence of only 0.5 vol% isopropanol, and a positive correlation between the H2O2 production and the K contents was found. The critical role of K was revealed as that K intercalation creates Lewis acidic sites for isopropanol adsorption and strengthens Lewis basic sites for hydrogen abstraction and proton release. The improved alcohol oxidation and enhanced O2 chemisorption synergistically result in dramatically accelerated PHOP over KTTCN. The findings provide the understanding of the preliminary active site dependent PHOP mechanism and bring insights for design of carbon nitride polymers with desirable photocatalytic performance.