Transition metal phosphosulfides (TMPSs) have shown great potential as efficient catalysts toward hydrogen evolution reaction (HER). To further understand and promote the catalytic activity at the phosphosulfide (PS) structures, the multifunctional role of TMPS needs to be explored. Herein, we report copper phosphosulfide (Cu₃P|S) coupled with graphene-like C₃N₄ (GL-C₃N₄) as an excellent HER photocatalyst with a hydrogen production rate of 8.78 mmol g⁻¹ h⁻¹ (20.22 mmol g⁻¹ h⁻¹ with 0.5 wt.% Pt). Systematic investigations on the interaction between Cu₃P|S and GL-C₃N₄ unveil that such impressive photocatalytic activity arises from the interfacial PN chemical bond that constructs a Z-scheme heterostructure. Time-resolved photoluminescence analysis indicates a considerably suppressed recombination rate of photoexcited charge carriers at the interface, which facilitates electron transfer and enhances the reducibility of electrons in the conduction band of Cu₃P|S. This work provides new design strategies for employing TMPSs as photocatalysts for highly efficient HER and other photoreduction reactions.

过渡金属磷硫化物（TMPS）已显示出巨大的潜力，可作为制氢反应（HER）的有效催化剂。为了进一步了解和促进在磷硫化物（PS）结构上的催化活性，需要探索TMPS的多功能作用。在此，我们报道了磷硫化铜（Cu ₃ P | S）与石墨烯状的C ₃ N ₄（GL-C ₃ N ₄）偶联，是一种优异的HER光催化剂，产氢率为8.78 mmol g ^-1  h ^-1（ 20.22 mmol g ^-1  h ^-1，含0.5 wt。％Pt）。对Cu ₃ P | S与GL-C ₃相互作用的系统研究N ₄揭示了这种令人印象深刻的光催化活性来自于构成Z型异质结构的界面P N化学键。时间分辨的光致发光分析表明，界面处的光激发电荷载流子的复合速率大大降低，这促进了电子转移并增强了Cu ₃ P | S导带中电子的可还原性。这项工作为采用TMPS作为高效HER和其他光还原反应的光催化剂提供了新的设计策略。