Ultrathin sulfur-doped holey carbon nitride nanosheets with superior photocatalytic hydrogen production from water

Abstract Surface engineering is an efficient way to enhance photoabsorption, promote charge separation and boost photocatalysis. Herein, sulfur-doped holey g-C3N4 nanosheets have been prepared through a universal self-templating approach with thiocyanuric acid as the single-precursor. By subtly controlling the feeding amount of precursor, the synthesized sulfur-doped holey g-C3N4 nanosheets exhibit excellent visible-light driven photocatalytic hydrogen production activity. The optimized catalyst presents a hydrogen evolution rate of 6225.4 μmol g−1h−1, with an apparent quantum yield of 10 % at 420 nm. Comprehensive characterizations and theoretical calculations suggest that the enhanced photocatalysis is attributed to the synergy of the enlarged surface area, the negatively-shifted conduction band, and the narrowed bandgap due to sulfur-doping and ultra-thin two-dimensional topology. This work highlights the importance of controlling the precursor dosage and inducing sulfur doping into the polymer, providing a promising and reliable strategy to simultaneously regulate the nanostructural and electronic structure of g-C3N4 for highly efficient photocatalysis.