Hydrothermally Induced Oxygen Doping of Graphitic Carbon Nitride with a Highly Ordered Architecture and Enhanced Photocatalytic Activity

As an amorphous or semicrystalline material, graphitic carbon nitride (g-C₃N₄) displays poor photocatalytic activity owing to rapid recombination of the photogenerated charge carriers, which is mainly caused by a high density of defects in the graphitic structure. In this work, a porous O-doped g-C₃N₄ (P-CNO) nanosheet with a highly ordered architecture is fabricated by introducing a novel hydrothermal treatment to the precursor before the final thermal condensation. The photocatalytic hydrogen evolution rate (HER) and HER per surface area of P-CNO are 13.9 and 1.7 times higher than that of bulk g-C₃N₄. The improved photocatalytic activity is ascribed to a synergistic effect of O doping, a porous sheet-like morphology, and increased crystallinity. This work also provides a new approach for the synthesis of other polymer-based photocatalysts with high crystallinity and excellent performance.