Rational design of modified donor-acceptor functionalized graphitic carbon nitride structures with tailored optoelectronic and textural features for visible light-assisted H2O2 production

Abstract

In this study, we tried to design novel structures of graphitic carbon nitride (GCN) by tuning the quantity of their structural NHx (x = 1, 2) and Ctriple bondN moieties via a facile NaBH4-assisted calcination of supramolecular assemblies of cyanuric acid and melamine (CM complex). These functional groups with different electron affinities would act as donor-acceptor (D-A) motifs in the obtained GCN conjugated polymer, constructing a simple analogy of a biomimetic D-A system. Consequently, the structurally modified sample (DCN) exhibited an extended electronic delocalization, and enhanced exciton dissociation owing to formation of the internal electric field in the molecular scale. Further, employing the CM complex endows the structures with an improved surface area and unique coral-like morphology. As a result, the modified sample showed a remarkable photocatalytic H2O2 production rate of 351 µmol h−1 g−1, which is much higher than that of 158 µmol h−1 g−1 for the pristine sample (CN).