物理化学学报 >> 2026, Vol. 42 >> Issue (9): 100332.doi: 10.1016/j.actphy.2026.100332

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氧空位介导的2D/2D Bi2MoO6/Bi2O2S S型异质结用于高效CO2光还原

殷鸿飞1,3,*(), 洪梦玲1, 张锦阳2, 王文涛2,*(), 陈伟4, 吴国志1,*()   

  1. 1 池州学院材料与环境工程学院, 安徽 池州 247000
    2 贵州师范学院, 贵州省固态电池关键材料与器件全省重点实验室, 贵州省纳米材料模拟与计算重点实验室, 贵州 贵阳 550018
    3 曲阜师范大学物理工程学院, 山东 曲阜 273165
    4 台州学院医药化工学院, 浙江 台州 318000
  • 收稿日期:2026-04-15 修回日期:2026-05-26 录用日期:2026-05-27 发布日期:2026-07-03
  • 通讯作者: Email: yinhf@czu.edu.cn (殷鸿飞)wtwang@gznc.edu.cn (王文涛)allen_0688@163.com (吴国志)

Oxygen vacancy-mediated 2D/2D Bi2MoO6/Bi2O2S S-scheme heterojunctions for efficient CO2 photoreduction

Hongfei Yin1,3,*(), Mengling Hong1, Jinyang Zhang2, Wentao Wang2,*(), Wei Chen4, Guozhi Wu1,*()   

  1. 1 School of Materials and Environmental Engineering, Chizhou University, Chizhou 247000, Anhui Province, China
    2 Guizhou Provincial Key Laboratory of Critical Materials and Devices for Solid-State Batteries, Guizhou Provincial Key Laboratory of Computational Nanomaterial Science, Guizhou Education University, Guiyang 550018, Guizhou Province, China
    3 School of Physics and Physical Engineering, Qufu Normal University, Qufu 273165, Shandong Province, China
    4 School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, Zhejiang Province, China
  • Received:2026-04-15 Revised:2026-05-26 Accepted:2026-05-27 Published:2026-07-03
  • Contact: Email: yinhf@czu.edu.cn (Hongfei Yin)wtwang@gznc.edu.cn (Wentao Wang)allen_0688@163.com (Guozhi Wu)

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摘要：

通过光催化高效还原CO2以生产高附加值化学品面临巨大挑战，主要体现在光催化剂的电荷分离与传输动力学以及CO2还原过程的热力学限制上。本研究提出了一种通过原位水热硫化法实现基于氧空位介导的二维/二维Bi2MoO6/Bi2O2S S型异质结的理性设计策略。X射线光电子能谱(XPS)和电子顺磁共振(EPR)测试证实，部分S2−取代[MoO4]2−形成了紧密结合的异质界面并诱导产生氧空位。密度泛函理论(DFT)计算表明，氧空位介导的Bi2MoO6/Bi2O2S S型异质结能显著降低*COOH形成这一决速步骤的能垒，从而优化CO2光还原热力学过程。实验结果表明，Bi2MoO6/Bi2O2S异质结(特别是BMOS5)具有最高的CO产率，达到11.01 μmol g−1 h−1，分别是纯相BMO和BOS的2.82倍与3.40倍。通过原位XPS、能带边缘测定及DFT计算，验证了S型电荷转移路径。这些研究结果为开发具有可调节缺陷的高性能S型异质结以实现太阳能驱动的二氧化碳还原提供了可行的途径。

关键词: S型异质结, 二氧化碳光还原, 电荷分离与转移动力学, 密度泛函理论

Abstract:

The efficient reduction of CO2 through photocatalysis to produce value-added chemicals faces considerable difficulties, particularly in relation to the charge separation and transfer kinetics of photocatalysts, along with the thermodynamics of the CO2 reduction process. Herein, we present a rational design of oxygen vacancy-mediated 2D/2D Bi2MoO6/Bi2O2S S-scheme heterojunctions via an in situ hydrothermal sulfidation strategy, where partial S2− substitution for [MoO4]2− forms a tightly bonded heterointerface and induces oxygen vacancies, as evidenced by X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) tests. Density functional theory (DFT) calculations reveal that the oxygen vacancy-mediated Bi2MoO6/Bi2O2S S-scheme heterojunction significantly lowers the energy barrier of *COOH formation rate-determining step, which in turn enhances the thermodynamics of CO2 photoreduction. Consequently, the Bi2MoO6/Bi2O2S heterojunctions, especially BMOS5, possessed the highest CO yield of 11.01 μmol g−1 h−1, corresponding to 2.82 and 3.40 times the yields of bare BMO and BOS. Based on in situ XPS, band edge determination, and DFT calculations, the S-scheme charge transfer pathway was verified. The findings provide a viable pathway toward developing high-performance S-scheme heterojunctions with tailored defects for solar-driven CO2 reduction.

Key words: S-scheme heterojunctions, CO2 photoreduction, Charge separation and transfer kinetics, Density functional theory