Subsurface oxygen defects electronically interacting with active sites on In2O3 for enhanced photothermocatalytic CO2 reduction

Weiqin Wei, Zhen Wei, Ruizhe Li, Zhenhua Li, Run Shi, Shuxin Ouyang (), Yuhang Qi, David Lee Philips and Hong Yuan
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Weiqin Wei: Central China Normal University
Zhen Wei: University of Hong Kong
Ruizhe Li: Central China Normal University
Zhenhua Li: Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences
Run Shi: Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences
Shuxin Ouyang: Central China Normal University
Yuhang Qi: Hebei University of Technology
David Lee Philips: University of Hong Kong
Hong Yuan: Central China Normal University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract Oxygen defects play an important role in many catalytic reactions. Increasing surface oxygen defects can be done through reduction treatment. However, excessive reduction blocks electron channels and deactivates the catalyst surface due to electron-trapped effects by subsurface oxygen defects. How to effectively extract electrons from subsurface oxygen defects which cannot directly interact with reactants is challenging and remains elusive. Here, we report a metallic In-embedded In2O3 nanoflake catalyst over which the turnover frequency of CO2 reduction into CO increases by a factor of 866 (7615 h−1) and 376 (2990 h−1) at the same light intensity and reaction temperature, respectively, compared to In2O3. Under electron-delocalization effect of O-In-(O)Vo-In-In structural units at the interface, the electrons in the subsurface oxygen defects are extracted and gather at surface active sites. This improves the electronic coupling with CO2 and stabilizes intermediate. The study opens up new insights for exquisite electronic manipulation of oxygen defects.

Date: 2022
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DOI: 10.1038/s41467-022-30958-5

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