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Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction
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Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction
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Journal Article
Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction
2021
Overview
The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO
2
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 CO
2
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 5
d
and S 2
p
orbits accelerates the photo-electrons transfer onto the surface, resulting in more electrons available for CO
2
reduction. As a result, the product generation rate of Au
SA
/Cd
1−x
S manifests a remarkable at least 113-fold enhancement compared with pristine Cd
1−x
S.
The electron density of reactive sites significantly affects catalytic performances. Here, authors demonstrate the electron density of different reactive sites can be modulated by regulating the type of vacancy and the size of Au, leading to effective CO
2
photoreduction.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
