Precisely tunable thickness of graphitic carbon nitride nanosheets for visible-light-driven photocatalytic hydrogen evolution.

Graphitic carbon nitride (GCN) nanosheets with unique physicochemical properties have received increasing attention in the area of photocatalysis, yet tunable thickness for the straightforward production of this graphite-like two-dimensional (2D) nanomaterial remains a challenge. In this work, GCN nanosheets with different thicknesses were firstly prepared by a direct calcination of melamine supramolecular aggregates (MSA) obtained from a hydrochloric acid (HCl)-induced hydrothermal assembly approach. The resultant nanosheets over nanometer scale thickness could be precisely controlled via simply adjusting the HCl concentration. Compared to the bulk GCN (BGCN), the thinner nanosheets possessed a high specific surface area, a large electronic-band structure, and fast charge separation ability. The thinnest nanosheets with a thickness of approximately 4 nm exhibited excellent visible-light-driven photocatalytic water splitting performance in hydrogen evolution (524 μmol h g), which is over 9-fold higher than the BGCN powder. This work provides a thickness-dependent strategy for the preparation of metal-free GCN nanosheets and develops a promising 2D photocatalyst for application in solar energy conversion.