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

引用本文: 殷鸿飞, 洪梦玲, 张锦阳, 王文涛, 陈伟, 吴国志. 氧空位介导的2D/2D Bi₂MoO₆/Bi₂O₂S S型异质结用于高效CO₂光还原[J]. 物理化学学报, 2026, 42(9): 100332. doi: 10.1016/j.actphy.2026.100332 shu

Citation: Hongfei Yin, Mengling Hong, Jinyang Zhang, Wentao Wang, Wei Chen, Guozhi Wu. Oxygen vacancy-mediated 2D/2D Bi₂MoO₆/Bi₂O₂S S-scheme heterojunctions for efficient CO₂ photoreduction[J]. Acta Physico-Chimica Sinica, 2026, 42(9): 100332. doi: 10.1016/j.actphy.2026.100332 shu

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.
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

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)

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:

English

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

Hongfei Yin ^{1, 3,
,} ,
Mengling Hong ^1, ,
Jinyang Zhang ^2, ,
Wentao Wang ^{2,
,} ,
Wei Chen ^4, ,
Guozhi Wu ^{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

Corresponding author: Email: yinhf@czu.edu.cn (Hongfei Yin); wtwang@gznc.edu.cn (Wentao Wang); allen_0688@163.com (Guozhi Wu)

Received Date: 15 April 2026
Accepted Date: 27 May 2026
Revised Date: 26 May 2026
Available Online: 15 September 2026

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

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沈阳化工大学材料科学与工程学院沈阳 110142

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

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)

English

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

Corresponding author: Email: yinhf@czu.edu.cn (Hongfei Yin); wtwang@gznc.edu.cn (Wentao Wang); allen_0688@163.com (Guozhi Wu)

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