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

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 C boolean AND N 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) ex-hibited 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 mu mol h-1 g-1, which is much higher than that of 158 mu mol h-1 g-1 for the pristine sample (CN).(c) 2022 Elsevier B.V. All rights reserved.

Automated summary

In this study, novel structures of graphitic carbon nitride (GCN) were designed by controlling the quantity of NHx(x = 1, 2) and C boolean AND N moieties through a facile NaBH4-assisted calcination of supramolecular assemblies of cyanuric acid and melamine (CM complex). These functional groups acted as donor-acceptor (D-A) motifs in the obtained GCN conjugated polymer, forming a biomimetic D-A system. The structurally modified sample (DCN) showed extended electronic delocalization and enhanced exciton dissociation, thanks to the formation of an internal electric field at the molecular scale. Furthermore, the CM complex endowed the structures with an improved surface area and unique coral-like morphology. As a result, the modified sample exhibited a remarkable photocatalytic H2O2 production rate of 351 μmol h-1 g-1, much higher than that of the pristine sample (CN).