Synergy of S doping and defect construction in holey ultra-thin g-C3N4 nanosheets for improved photocatalytic hydrogen production from water

Combining the advantages of multiple strategies including morphology control, atom doping, and defect construction, the photocatalytic hydrogen evolution reaction (HER) performance of graphitic carbon nitride (g-C 3 N 4 ) may be boosted significantly. Herein, holey ultra-thin g-C 3 N 4 nanosheets (CNS-x, x = H, O, N) modified with structural vacancies and sulfur (S) dopant are synthesized through a straightforward method involving the pyrolysis of thiocyanuric acid under various gas atmospheres. The textural properties, type and concentration of structural defect, and S doping level are significantly influenced by the gas atmosphere. Remarkably, CNS-H with C, N dual defects and S-dopant exhibits the HER rate of 46.59 mmol·g −1 ·h −1 , which is 16.68 times higher than that of bulk g-C 3 N 4 . The corresponding apparent quantum yields are 17.24 % at 420 nm and 1.90 % at 520 nm. The enhanced HER performance of CNS-H can be attributed to the combined effect of improved charge separation, extended photoabsorption, and optimized properties of the platinum cocatalyst.