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Excited Electron-Rich Bi~((3–x)+) Sites: A Quantum Well-Like Structure for Highly Promoted Selective Photocatalytic CO_2 Reduction Performance

机译:Excited Electron-Rich Bi~((3–x)+) Sites: A Quantum Well-Like Structure for Highly Promoted Selective Photocatalytic CO_2 Reduction Performance

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摘要

Most of the current research on the photocatalytic mechanism ofsemiconductors is still on the simulation and evaluation of ground-stateactive sites. Insights into photogenerated electron transition paths andexcited-state active sites during photocatalysis are still insufficient. Herein,combining femtosecond time-resolved transient absorption spectroscopy, insitu Fourier-transform infrared spectroscopy, synchronous illumination X-rayphotoelectron spectroscopy, and theoretical calculation results rationallyreveal that in complex bimetallic oxyhalides the ultrathin rich oxygenvacancies (ROV) PbBiO_2Cl (PBOC) double unit cell (DUC) layers facilitatemigration and separation of photogenerated electrons from the bulk to Bisites near the surface oxygen vacancies (OVs), then form the excited electronrichBi~((3–x)+) sites like quantum well structure. The excited Bi~((3–x)+) sites actas wells for photogenerated electrons leading to lower energy barrier in therate determining step for the formation of *CO from *COOH intermediate.Without photosensitizers and sacrificial agents, ROV DUC PBOC exhibit highCO generation rate (16.02 μmol h~(–1) g~(–1)) that is 18 times higher than that ofbulk PBOC. In situ characterization combined with theoretical calculationprovides effective insight into the photocatalytic mechanism of photoexcitedsemiconductor materials.

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  • 来源
    《Advanced functional materials》 |2022年第35期|2202885.1-2202885.11|共11页
  • 作者单位

    School of Chemistry and Chemical EngineeringInstitute for Energy ResearchJiangsu University301 Xuefu Road, Zhenjiang 212013, P. R. China;

    School of Chemistry and Chemical EngineeringInstitute for Energy ResearchJiangsu University301 Xuefu Road, Zhenjiang 212013, P. R. China Department of PhysicsDepartment of Materials Science and Engineeringand Department of Biomedical EngineeringCity Unive;

    Beijing National Laboratory for Condensed Matter PhysicsCAS Key Laboratory of Soft Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190, P. R. ChinaDepartment of PhysicsDepartment of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongKowloon, Hong Kong, P. R. China;

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  • 原文格式 PDF
  • 正文语种 英语
  • 中图分类
  • 关键词

    CO_2 reduction; oxygen vacancies; PbBiO_2Cl; photocatalysts; quantum wells;

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