Spatiotemporal imaging of charge transfer in photocatalyst particles

Ruotian Chen, Zefeng Ren, Yu Liang, Guanhua Zhang, Thomas Dittrich, Runze Liu, Yang Liu, Yue Zhao, Shan Pang, Hongyu An, Chenwei Ni, Panwang Zhou, Keli Han, Fengtao Fan () and Can Li ()
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Ruotian Chen: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Zefeng Ren: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yu Liang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Guanhua Zhang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Thomas Dittrich: Helmholtz-Center Berlin for Materials and Energy GmbH
Runze Liu: Institute of Frontier and Interdisciplinary Science, Shandong University
Yang Liu: Institute of Frontier and Interdisciplinary Science, Shandong University
Yue Zhao: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Shan Pang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Hongyu An: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Chenwei Ni: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Panwang Zhou: Institute of Frontier and Interdisciplinary Science, Shandong University
Keli Han: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Fengtao Fan: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Can Li: Dalian Institute of Chemical Physics, Chinese Academy of Sciences

Nature, 2022, vol. 610, issue 7931, 296-301

Abstract: Abstract The water-splitting reaction using photocatalyst particles is a promising route for solar fuel production1–4. Photo-induced charge transfer from a photocatalyst to catalytic surface sites is key in ensuring photocatalytic efficiency5; however, it is challenging to understand this process, which spans a wide spatiotemporal range from nanometres to micrometres and from femtoseconds to seconds6–8. Although the steady-state charge distribution on single photocatalyst particles has been mapped by microscopic techniques9–11, and the charge transfer dynamics in photocatalyst aggregations have been revealed by time-resolved spectroscopy12,13, spatiotemporally evolving charge transfer processes in single photocatalyst particles cannot be tracked, and their exact mechanism is unknown. Here we perform spatiotemporally resolved surface photovoltage measurements on cuprous oxide photocatalyst particles to map holistic charge transfer processes on the femtosecond to second timescale at the single-particle level. We find that photogenerated electrons are transferred to the catalytic surface quasi-ballistically through inter-facet hot electron transfer on a subpicosecond timescale, whereas photogenerated holes are transferred to a spatially separated surface and stabilized through selective trapping on a microsecond timescale. We demonstrate that these ultrafast-hot-electron-transfer and anisotropic-trapping regimes, which challenge the classical perception of a drift–diffusion model, contribute to the efficient charge separation in photocatalysis and improve photocatalytic performance. We anticipate that our findings will be used to illustrate the universality of other photoelectronic devices and facilitate the rational design of photocatalysts.

Date: 2022
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DOI: 10.1038/s41586-022-05183-1

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