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  • 标题:Single-molecule and -particle probing crystal edge/corner as highly efficient photocatalytic sites on a single TiO2 particle
  • 本地全文:下载
  • 作者:Wei-Kang Wang ; Wei-Kang Wang ; Jie-Jie Chen
  • 期刊名称:Proceedings of the National Academy of Sciences
  • 印刷版ISSN:0027-8424
  • 电子版ISSN:1091-6490
  • 出版年度:2019
  • 卷号:116
  • 期号:38
  • 页码:18827-18833
  • DOI:10.1073/pnas.1907122116
  • 出版社:The National Academy of Sciences of the United States of America
  • 摘要:The exposed active sites of semiconductor catalysts are essential to the photocatalytic energy conversion efficiency. However, it is difficult to directly observe such active sites and understand the photogenerated electron/hole pairs’ dynamics on a single catalyst particle. Here, we applied a quasi-total internal reflection fluorescence microscopy and laser-scanning confocal microscopy to identify the photocatalytic active sites at a single-molecule level and visualized the photogenerated hole–electron pair dynamics on a single TiO 2 particle, the most widely used photocatalyst. The experimental results and density functional theory calculations reveal that holes and electrons tend to reach and react at the same surface sites, i.e., crystal edge/corner, within a single anatase TiO 2 particle owing to the highly exposed (001) and (101) facets. The observation provides solid proof for the existence of the surface junction “edge or corner” on single TiO 2 particles. These findings also offer insights into the nature of the photocatalytic active sites and imply an activity-based strategy for rationally engineering catalysts for improved photocatalysis, which can be also applied for other catalytic materials..
  • 关键词:photocatalyst ; TiO 2 ; single;molecule microscopy ; single;particle microscopy ; crystal edge;corner
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