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.

表面工程是增强光吸收，促进电荷分离和促进光催化的有效方法。在本文中，已经通过使用硫氰尿酸作为单一前体的通用自模板方法制备了硫掺杂的多孔gC ₃ N ₄纳米片。通过巧妙地控制前体的进料量，合成的硫掺杂有孔gC ₃ N ₄纳米片表现出优异的可见光驱动的光催化制氢活性。经过优化的催化剂的析氢速率为6225.4μmolg ^-1 h ^-1，在420 nm下的表观量子产率为10％。综合表征和理论计算表明，增强的光催化作用归因于由于硫掺杂和超薄二维拓扑结构而导致的表面积增加，负迁移带和窄带隙的协同作用。这项工作强调了控制前体剂量并在聚合物中引入硫的重要性，这为同时调节gC ₃ N ₄的纳米结构和电子结构提供了一种有前途且可靠的策略，以实现高效的光催化作用。