S型SnO<sub>2</sub>/BiOBr异质结光催化还原CO<sub>2</sub>的电荷传输机理

引用本文: 安月皎, 刘文暄, 张艳峰, 张建军, 路战胜. S型SnO₂/BiOBr异质结光催化还原CO₂的电荷传输机理[J]. 物理化学学报, 2024, 40(12): 240702. doi: 10.3866/PKU.WHXB202407021 shu

Citation: Yuejiao An, Wenxuan Liu, Yanfeng Zhang, Jianjun Zhang, Zhansheng Lu. Revealing Photoinduced Charge Transfer Mechanism of SnO₂/BiOBr S-Scheme Heterostructure for CO₂ Photoreduction[J]. Acta Physico-Chimica Sinica, 2024, 40(12): 240702. doi: 10.3866/PKU.WHXB202407021 shu

S型SnO₂/BiOBr异质结光催化还原CO₂的电荷传输机理

安月皎 ^{1, †,} ,
刘文暄 ^{2, †,} ,
张艳峰 ^{1,
,} ,
张建军 ^{3,
,} ,
路战胜 ^{4, 2,
,}

1.
河北师范大学化学与材料科学学院, 无机纳米材料河北省重点实验室, 国家实验化学教学示范中心, 石家庄 050024
2.
河南师范大学物理学院, 河南省先进半导体与功能器件集成重点实验室, 河南新乡 453007
3.
中国地质大学(武汉)材料与化学学院太阳燃料实验室, 武汉 430078
4.
北京化工大学数理学院, 北京 100029

通讯作者: 张艳峰, zhangyanfeng@hebtu.edu.cn; 张建军, zhangjianjun@cug.edu.cn; 路战胜, zslu@buct.edu.cn

基金项目:
国家自然科学基金项目 12274118

国家自然科学基金项目 52202375

河北省自然科学基金 B2020205013

河北省自然科学基金 B2022205008

河北师范大学科技项目 L2021K01

河北省创新能力提升计划项目 22567604H

河南省杰出外籍科学家工作室 GZS2023007

河南省高等学校重点科研项目计划基础研究专项 22ZX013
^†These authors contributed equally to this work.

摘要: S型异质结可以实现光生载流子有效空间分离，保持较强的氧化还原能力。因此，深入了解S型异质结构的光致电荷转移动力学对提高其光催化性能至关重要。本文采用原位水热法制备了紧密接触的SnO₂/BiOBr S型异质结。优化后的SnO₂/BiOBr具有优异的光催化CO₂还原性能，CO和CH₄的产率分别为345.7和6.7 μmol·g^–1·h^–1，分别是纯BiOBr的5.6和3.7倍。利用原位XPS和飞秒瞬态吸收光谱(fs-TA)表征了SnO₂/BiOBr S型异质结的光致电荷转移机制和动力学。发现光生载流子出现了新的拟合寿命，这可归因于S型异质结的界面电子转移，进一步证明了光电子从SnO₂导带到BiOBr价带的超快转移通道。因此，BiOBr导带中的还原电子和SnO₂价带中的氧化空穴得以保留。本研究对S型异质结的光致电荷传输机理提供了更深刻的理解。

关键词:

English

Revealing Photoinduced Charge Transfer Mechanism of SnO₂/BiOBr S-Scheme Heterostructure for CO₂ Photoreduction

1.
National Demonstration Center for Experimental Chemistry Education, Hebei Key Laboratory of Inorganic Nano-materials, College of Chemistry and Materials Science, Hebei Normal University, Shijiazhuang 050024, China
2.
School of Physics, Henan Key Laboratory of Advanced Semiconductor & Functional Device Integration, Henan Normal University, Xinxiang 453007, Henan Province, China
3.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, China
4.
School of Mathematics and Physics, Beijing University of Chemical Technology, Beijing 100029, China

Corresponding author: Email: zhangyanfeng@hebtu.edu.cn (Y.Z.); Email: zhangjianjun@cug.edu.cn (J.Z.); Email: zslu@buct.edu.cn (Z.L.)

Received Date: 23 July 2024
Accepted Date: 22 August 2024
Revised Date: 21 August 2024
Available Online: 15 December 2024
Fund Project:
National Natural Science Foundation of China

National Natural Science Foundation of China

Natural Science Foundation of Hebei of China

Natural Science Foundation of Hebei of China

Science and Technology Project of Hebei Normal University of China

Innovation Capability Improvement Plan Project of Hebei Province

Henan Center for Outstanding Overseas Scientists

Special Project for Fundamental Research in University of Henan Province

Abstract: S-scheme heterojunctions can preserve strong redox capacity on the basis of achieving spatial separation of photogenerated carriers. Therefore, a deep comprehension of the photoinduced charge transfer dynamics in S-scheme heterostructures is vital to enhancing photocatalytic properties. Herein, SnO₂/BiOBr S-scheme heterojunctions with tight contact are fabricated with in situ hydrothermal method. The optimal SnO₂/BiOBr exhibits excellent photocatalytic performance for CO₂ reduction, with yields of CO and CH₄ of 345.7 and 6.7 μmol∙g^–1∙h^–1, which are 5.6 and 3.7 times higher than those of the original BiOBr. The photoinduced charge transfer mechanism and dynamics of SnO₂/BiOBr S-scheme heterostructure are characterized by in situ X-ray photoelectron spectrum (XPS) and femtosecond transient absorption spectroscopy (fs-TA). A new fitted lifetime of photogenerated carriers are observed, which could be attributed to interfacial electron transfer of S-scheme heterojunction, further illustrating an ultrafast transfer channel for photoelectrons from SnO₂ conduction band to BiOBr valence band. As a result, the powerful reduced electrons in BiOBr conduction band and the powerful oxidation holes in SnO₂ valence band are retained. This work provides profound comprehension of photoinduced charge transfer mechanism of S-scheme heterojunction.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

S型SnO₂/BiOBr异质结光催化还原CO₂的电荷传输机理

通讯作者: 张艳峰, zhangyanfeng@hebtu.edu.cn; 张建军, zhangjianjun@cug.edu.cn; 路战胜, zslu@buct.edu.cn

English

Revealing Photoinduced Charge Transfer Mechanism of SnO₂/BiOBr S-Scheme Heterostructure for CO₂ Photoreduction

Corresponding author: Email: zhangyanfeng@hebtu.edu.cn (Y.Z.); Email: zhangjianjun@cug.edu.cn (J.Z.); Email: zslu@buct.edu.cn (Z.L.)

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Revealing Photoinduced Charge Transfer Mechanism of SnO2/BiOBr S-Scheme Heterostructure for CO2 Photoreduction

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