Gas bubbling exfoliation strategy towards 3D g-C3N4 hierarchical architecture for superior photocatalytic H2 evolution

Graphitic carbon nitride (g-C3N4) shows a graphite-like layered structure, which provides a high theoretical value for solar-to-hydrogen evolution especially for a 2D nanostructure. However, conventional poly condensation induces a strong agglomeration and collapse of nanostructure, resulting in a relatively poor photocatalytic performance. To overcome this problem, we develop a gas bubbling exfoliation strategy with NH4Cl assistant to make ultrathin 2D g-C3N4 nanosheets self-assembled into a 3D macroporous network on a large scale. The hierarchical structure significantly improves the specific surface area to 176.4 m(2) g(-1) (11.6 times higher than the reference g-C3N4), which allows a large water/g-C3N4 interface for photocatalytic water reduction reaction. The ultrathin 2D g-C3N4 nanosheets show a thickness of about 1.4 nm, which greatly suppress photoinduced carriers recombination and enhance charge transfer at the interface. Furthermore, the doping of N and Cl is achieved during synthesis. As a result, the resulting g-C3N4 demonstrates a remarkable improvement in H-2 production of 12.89 mmol g(-1) h(-1), which is 21 times higher than the g-C3N4 obtained from the conventional condensation method. These explorations provide a facile guidance for the quasi 3D g-C3N4 hierarchical architecture engineering even for various energy-related applications.(c) 2022 Elsevier B.V. All rights reserved.

Automated summary

In this study, ultra-thin 2D g-C3N4 nanosheets were successfully self-assembled into a large-scale 3D macroporous structure with the assistance of NH4Cl through a gas bubbling exfoliation strategy. The doping of N and Cl was achieved during synthesis. The resulting hierarchical structure exhibited remarkable improvement in photocatalytic water reduction reaction.