物理化学学报 >> 2026, Vol. 42 >> Issue (6): 100244.doi: 10.1016/j.actphy.2026.100244

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双功能单原子修饰SnS2/CdS S型光催化剂用于协同产氢与乳酸氧化的DFT研究

袁成成1, 夏伟1,*(), 王骏2, 朱潇锋2, 张勇3, 朱必成1,2,*(), 余家国1,*()   

  1. 1 中国地质大学(武汉)材料与化学学院, 太阳燃料实验室, 湖北 武汉 430078
    2 西南科技大学材料与化学学院, 环境友好能源材料国家重点实验室, 四川 绵阳 621010
    3 湖北理工学院新材料与绿色化工学院，高分子材料化学助剂湖北省工程研究中心，湖北 黄石 435003
  • 收稿日期:2026-01-02 修回日期:2026-01-10 录用日期:2026-01-15 发布日期:2026-04-21
  • 通讯作者: Email: xiawei@cug.edu.cn (夏伟)zhubicheng@cug.edu.cn (朱必成)yujiaguo93@cug.edu.cn (余家国)

A dual-functional single-atom modified SnS2/CdS S-scheme photocatalyst for synergistic hydrogen production and lactic acid oxidation: A DFT study

Chengcheng Yuan1, Wei Xia1,*(), Jun Wang2, Xiaofeng Zhu2, Yong Zhang3, Bicheng Zhu1,2,*(), Jiaguo Yu1,*()   

  1. 1 Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China
    2 State Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang 621010, Sichuan Province, China
    3 School of Advanced Materials and Green Chemical Engineering, Hubei Engineering Research Center for Chemical Additives of Polymer Materials, Hubei Polytechnic University, Huangshi 435003, Hubei Province, China
  • Received:2026-01-02 Revised:2026-01-10 Accepted:2026-01-15 Published:2026-04-21
  • Contact: Email: xiawei@cug.edu.cn (Wei Xia)zhubicheng@cug.edu.cn (Bicheng Zhu)yujiaguo93@cug.edu.cn (Jiaguo Yu)

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摘要：

设计高效S型光催化剂以实现同步产氢与有机物氧化，对于可持续能源转化具有重要意义。本文构建了一种负载过渡金属单原子(TM = Pt、Pd、Au)的新型SnS2/CdS S型异质结。通过系统的密度泛函理论(DFT)计算，研究了其几何结构、电子性质以及表面氢吸附与乳酸(LA)氧化反应机制。结果表明，在异质结中电子通过界面Cd–S键从CdS向SnS2转移，形成稳定的复合结构，而TM单原子通过与表面S原子形成TM–S键得以稳定。TM原子的引入增强了界面电子转移。值得注意的是，锚定在CdS表面的TM原子可有效调控相邻S原子的p带中心，从而弱化S–H键并优化氢吸附-脱附平衡；同时，SnS2表面的TM原子能增强LA吸附能，降低脱氢氧化过程中决速步骤的能垒。该工作证明，在S型异质结的不同组分上策略性排布单原子可协同增强还原与氧化半反应，为合理设计高性能单原子负载S型光催化体系以实现协同产氢与高值化学品合成提供了深刻见解。

关键词: S型异质结, 金属单原子, 电子转移, 氢吸附, 乳酸氧化

Abstract:

Designing efficient S-scheme photocatalysts for simultaneous H2 evolution and organic oxidation is highly desirable for sustainable energy conversion. Herein, a novel SnS2/CdS S-scheme heterojunction loaded with transition metal single atoms (TM = Pt, Pd, Au) was constructed. Systematic density functional theory (DFT) calculations are performed to investigate the geometric structure, electronic properties, and the mechanisms of surface H adsorption and lactic acid (LA) oxidation reactions. The results reveal that in the heterojunction, electrons transfer from CdS to SnS2 through interfacial Cd–S bonds, forming a stable composite structure, while the TM single atoms are stabilized by forming TM–S bonds with surface S atoms. The incorporation of TM atoms enhances the interfacial electron transfer. Notably, the TM atoms anchored on the CdS surface effectively modulate the p-band center of neighboring S atoms, thereby weakening the S–H bond and optimizing the H adsorption-desorption equilibrium. Concurrently, those on the SnS2 surface enhance the adsorption energy of LA and reduce the energy barrier of the rate-determining step in the dehydrogenation oxidation process. This work demonstrates that the strategic placement of single atoms on different components of an S-scheme heterojunction can synergistically enhance both the reduction and oxidation half-reactions, offering profound insights for the rational design of high-performance single-atom-loaded S-scheme photocatalytic systems for cooperative H2 production and value-added chemical synthesis.

Key words: S-scheme heterojunctions, Metal single atoms, Electron transfer, Hydrogen adsorption, Lactic acid oxidation