Construction of structural defects in photocatalysts is a powerful tool for regulating their photocatalytic performance. In this work, we develop a facile one-step coupling cold plasma and thermal polymerization approach to synthesize a series of nitrogen defect-rich graphitic carbon nitrides (C₃N_4-x), which are used for visible-light-driven hydrogen generation from water. The nitrogen defect-induced band structure regulation of C₃N_4-x catalysts can be carried out through controlling the bombardment time and excitation power of generator during the plasma modification process. The defective C₃N_4-x catalysts have the extended visible light absorption and improved separation efficiency of photogenerated charge carriers, which results in the boosted hydrogen generation activity. Particularly, the optimal C₃N_4-x possesses a hydrogen generation rate of 2.46 mmol h⁻¹ g⁻¹, which is about 4.5 times higher than the pristine C₃N₄ synthesized by the single thermal polymerization of urea. The cold plasma modification-based one-step synthesis approach guides us for rationally designing defective nanomaterials with excellent catalytic performance.

光催化剂中结构缺陷的构建是调节其光催化性能的有力工具。在这项工作中，我们开发了一种简便的单步耦合冷等离子体和热聚合方法，以合成一系列富氮缺陷的石墨碳氮化物（C ₃ N _4-x），用于可见光驱动的制氢从水。通过控制等离子体改性过程中发生器的轰击时间和激发功率，可以进行氮缺陷引起的C ₃ N _4-x催化剂的能带结构调节。有缺陷的C ₃ N _4-x催化剂具有扩展的可见光吸收能力和提高了光生载流子的分离效率，从而提高了氢的产生活性。特别地，最佳的C ₃ N _4-x具有2.46mmol h ^-1  g ^-1的氢生成速率，这是通过尿素的单热聚合合成的原始C ₃ N _4的约4.5倍。基于冷等离子体改性的一步合成方法指导我们合理设计具有优异催化性能的有缺陷的纳米材料。