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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 ,  夏伟 ,  王骏 ,  朱潇锋 ,  张勇 ,  朱必成 ,  余家国

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引用本文: 袁成成, 夏伟, 王骏, 朱潇锋, 张勇, 朱必成, 余家国. 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[J]. 物理化学学报, 2026, 42(6): 100244. doi: 10.1016/j.actphy.2026.100244 shu
Citation:  Chengcheng Yuan,  Wei Xia,  Jun Wang,  Xiaofeng Zhu,  Yong Zhang,  Bicheng Zhu,  Jiaguo Yu. A dual-functional single-atom modified SnS2/CdS S-scheme photocatalyst for synergistic hydrogen production and lactic acid oxidation: A DFT study[J]. Acta Physico-Chimica Sinica, 2026, 42(6): 100244. doi: 10.1016/j.actphy.2026.100244 shu

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

  • 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

    • 通讯作者: 夏伟,E-mail:xiawei@cug.edu.cn; 朱必成,E-mail:zhubicheng@cug.edu.cn; 余家国,E-mail:yujiaguo93@cug.edu.cn
  • 基金项目:

    本研究得到国家自然科学基金(52173065,U24A2071,52372294,22361142704和22238009)；环境友好能源材料国家重点实验室开放基金(24kfhg05)；以及湖北省自然科学基金黄石创新发展联合基金重点项目(2025AFD004)资助

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。

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