物理化学学报 >> 2024, Vol. 40 >> Issue (12): 2407021.doi: 10.3866/PKU.WHXB202407021

所属专题: 太阳燃料制备

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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. 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
  • 收稿日期:2024-07-23 修回日期:2024-08-21 录用日期:2024-08-22 发布日期:2024-09-02
  • 通讯作者: Email: zhangyanfeng@hebtu.edu.cn (张艳峰)zslu@buct.edu.cn (路战胜)zhangjianjun@cug.edu.cn (张建军)
  • 作者简介:

    †These authors contributed equally to this work.

  • 基金资助:
    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)

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

Yuejiao An1, Wenxuan Liu2, Yanfeng Zhang1,*(), Jianjun Zhang3,*(), Zhansheng Lu4,2,*()   

  1. 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
  • Received:2024-07-23 Revised:2024-08-21 Accepted:2024-08-22 Published:2024-09-02
  • Contact: Email: zhangyanfeng@hebtu.edu.cn (Yanfeng Zhang)zslu@buct.edu.cn (Zhansheng Lu)zhangjianjun@cug.edu.cn (Jianjun Zhang)
  • Supported by:
    National Natural Science Foundation of China(12274118); National Natural Science Foundation of China(52202375); Natural Science Foundation of Hebei of China(B2020205013); Natural Science Foundation of Hebei of China(B2022205008); Science and Technology Project of Hebei Normal University of China(L2021K01); Innovation Capability Improvement Plan Project of Hebei Province(22567604H); Henan Center for Outstanding Overseas Scientists(GZS2023007); Special Project for Fundamental Research in University of Henan Province(22ZX013)

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: SnO2/BiOBr, 光催化还原二氧化碳, S型异质结, fs-TA, 原位XPS

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: SnO2/BiOBr, CO2 photoreduction, S-scheme heterojunction, fs-TA, in situ XPS