Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

Yuehan Cao, Lan Guo, Meng Dan, Dmitry E. Doronkin, Chunqiu Han, Zhiqiang Rao, Yang Liu, Jie Meng, Zeai Huang, Kaibo Zheng, Peng Chen, Fan Dong and Ying Zhou ()
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Yuehan Cao: Southwest Petroleum University
Lan Guo: Southwest Petroleum University
Meng Dan: Southwest Petroleum University
Dmitry E. Doronkin: Institute for Chemical Technology and Polymer Chemistry and Institute of Catalysis Research and Technology, Karlsruhe Institute of Technology
Chunqiu Han: Southwest Petroleum University
Zhiqiang Rao: Southwest Petroleum University
Yang Liu: Southwest Petroleum University
Jie Meng: Lund University
Zeai Huang: Southwest Petroleum University
Kaibo Zheng: Lund University
Peng Chen: Southwest Petroleum University
Fan Dong: University of Electronic Science and Technology of China
Ying Zhou: Southwest Petroleum University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO2 reduction reaction, which involves multi-electron participation in the conversion process. Herein, we propose a conceptually different mechanism for surface electron density modulation based on the model of Au anchored CdS. We firstly manipulate the direction of electron transfer by regulating the vacancy types of CdS. When electrons accumulate on vacancies instead of single Au atoms, the adsorption types of CO2 change from physical adsorption to chemical adsorption. More importantly, the surface electron density is manipulated by controlling the size of Au nanostructures. When Au nanoclusters downsize to single Au atoms, the strong hybridization of Au 5d and S 2p orbits accelerates the photo-electrons transfer onto the surface, resulting in more electrons available for CO2 reduction. As a result, the product generation rate of AuSA/Cd1−xS manifests a remarkable at least 113-fold enhancement compared with pristine Cd1−xS.

Date: 2021
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DOI: 10.1038/s41467-021-21925-7

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