The options of transition metals as co-catalysts for photocatalytic H₂S splitting are restricted to some noble metals and related compounds which have noticeable achievements despite their high prices. Substituting with cheap transition metals and downsizing the size to single atom level are economic ways to lower the cost. Herein, the s-triazine graphite-like carbon nitride sheet g-C₃N₄ (001) is chosen as the model to study the performances of 3d and 4d transition metal single atoms (TMSA = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, Cd) in H₂S splitting based on density functional theory (DFT) calculations. It is found that low-cost transition metals with industrial relevance (Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Zr, Nb, Mo, Tc, Cd) are completely comparable with noble metals (Ru, Rh, Pd, Ag). Among them, V and Nb are the most promising co-catalysts with good thermodynamic stabilities, favorable responses to visible light, high photoinduced electron-hole separation efficiencies, sufficient potentials for H₂S splitting, and low energy barriers for H₂S dissociation into H₂ and S. The noticeable improved activities of V/g-C₃N₄ and Nb/g-C₃N₄ are attributed to the formation of strong interfacial chemical bonds which could promote electrons transferring to H₂S derivates. In addition, the introduction of photoinduced electrons could further improve the activities of V/g-C₃N₄ and Nb/g-C₃N₄ with more electrons transferring to H₂S derivates. It is expected that this work could provide a helpful guidance to choose appropriate TMSA co-catalysts as references for H₂S splitting.

过渡金属作为光催化分解H ₂ S的助催化剂的选择仅限于某些贵金属和相关化合物，尽管价格昂贵，但它们仍取得了显著成就。用便宜的过渡金属代替并将尺寸减小到单个原子水平是降低成本的经济方法。本文以s-三嗪类石墨氮化碳片gC ₃ N ₄（001）为模型，研究3d和4d过渡金属单原子（TMSA = Sc，Ti，V，Cr，Mn，Fe ，Co，Ni，Cu，Zn，Y，Zr，Nb，Mo，Tc，Ru，Rh，Pd，Ag，Cd）在H _2中基于密度泛函理论（DFT）计算的S分裂。发现具有工业相关性的低成本过渡金属（Ti，V，Cr，Mn，Fe，Co，Ni，Cu，Zn，Zr，Nb，Mo，Tc，Cd）与贵金属（Ru， Rh，Pd，Ag）。其中，V和Nb是最有前途的助催化剂具有良好的热力学稳定性，可见光，高光诱导的电子-空穴的分离效率，足够的电位用于h有利反应₂小号分裂，和低能量壁垒用于h ₂离解常数为H ₂和S。V/ gC ₃ N ₄和Nb / gC ₃ N ₄的明显改善的活性归因于牢固的界面化学键的形成，其可以促进电子转移至H ₂ S衍生物。另外，引入更多的电子转移至H ₂ S衍生物中，引入光诱导电子可以进一步提高V / gC ₃ N ₄和Nb / gC ₃ N ₄的活性。期望这项工作可以为选择合适的TMSA助催化剂提供参考，以作为H ₂ S裂解的参考。