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Photocatalytic water oxidation is a crucial step in water splitting, but is generally restricted by the slow kinetics. Therefore, it is necessary to develop high-performance water oxidation photocatalysts. Herein, the Fe-doped Bi2WO6 nanosheets with oxygen vacancies (OVs) were synthesized for enhanced photocatalytic water oxidation efficiency, showing a synergistic effect between Fe dopants and OVs. When a molar fraction of 2% Fe was doped into the Bi2WO6 nanosheets, the visible-light-driven photocatalytic oxygen evolution rate was increased up to 131.3 µmol·h−1·gcat−1 under ambient conditions, which was more than 3 times that of pure Bi2WO6 nanosheets. The proper doping concentration of Fe could promote the formation of OVs and at the same time modulate the band structure of catalysts, especially the position of the valence band maximum (VBM), leading to effective visible-light absorption and enhanced oxidizing ability of photogenerated holes. With ameliorated localized electron distribution, fast charge transfer channel emerged between the OVs and adjacent metal atoms, which accelerated the charge carrier transfer and promoted the separation of photoexcited electrons and holes. This work provides feasible approaches for designing efficient two-dimensional semiconductor water oxidation photocatalysts that could utilize visible-light, which will make more use of solar energy.


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Constructing charge transfer channel between dopants and oxygen vacancies for enhanced visible-light-driven water oxidation

Show Author's information Ming Cheng1Lan Yang1Huiyi Li1Wei Bai1Chong Xiao1,2( )Yi Xie1,2( )
Hefei National Laboratory for Physical Sciences at the Microscale,CAS Centre for Excellence in Nanoscience, iCHEM, University of Science and Technology of China,Hefei,230026,China;
Institute of Energy,Hefei Comprehensive National Science Center,Hefei,230031,China;

Abstract

Photocatalytic water oxidation is a crucial step in water splitting, but is generally restricted by the slow kinetics. Therefore, it is necessary to develop high-performance water oxidation photocatalysts. Herein, the Fe-doped Bi2WO6 nanosheets with oxygen vacancies (OVs) were synthesized for enhanced photocatalytic water oxidation efficiency, showing a synergistic effect between Fe dopants and OVs. When a molar fraction of 2% Fe was doped into the Bi2WO6 nanosheets, the visible-light-driven photocatalytic oxygen evolution rate was increased up to 131.3 µmol·h−1·gcat−1 under ambient conditions, which was more than 3 times that of pure Bi2WO6 nanosheets. The proper doping concentration of Fe could promote the formation of OVs and at the same time modulate the band structure of catalysts, especially the position of the valence band maximum (VBM), leading to effective visible-light absorption and enhanced oxidizing ability of photogenerated holes. With ameliorated localized electron distribution, fast charge transfer channel emerged between the OVs and adjacent metal atoms, which accelerated the charge carrier transfer and promoted the separation of photoexcited electrons and holes. This work provides feasible approaches for designing efficient two-dimensional semiconductor water oxidation photocatalysts that could utilize visible-light, which will make more use of solar energy.

Keywords: oxygen vacancies, water oxidation reaction, Bi2WO6 nanosheets, valence band maximum, charge transfer channel

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Publication history
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Acknowledgements

Publication history

Received: 11 March 2021
Revised: 17 May 2021
Accepted: 19 May 2021
Published: 04 June 2021
Issue date: October 2021

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© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

This work was financially supported by the National Key R & D Program of China (No. 2017YFA0207301), the National Natural Science Foundation of China (Nos. 21622107, 11621063, U1532265, and 21890750), the Youth Innovation Promotion Association CAS (No. 2016392), the Key Research Program of Frontier Sciences (No. QYZDY-SSW-SLH011), and the Major Program of Development Foundation of Hefei Center for Physical Science and Technology (No. 2017FXZY003).

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