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

Cao, Yuehan ; Guo, Lan ; Dan, Meng LU ; Doronkin, Dmitry E. ; Han, Chunqiu ; Rao, Zhiqiang ; Liu, Yang ; Meng, Jie ; Huang, Zeai and Zheng, Kaibo LU , et al. (2021) In Nature Communications 12(1).
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... (More)

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.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
12
issue
1
article number
1675
publisher
Nature Publishing Group
external identifiers
  • pmid:33723264
  • scopus:85102519602
ISSN
2041-1723
DOI
10.1038/s41467-021-21925-7
language
English
LU publication?
yes
id
3b8c559a-e453-495d-b7ba-5321c9a15d1a
date added to LUP
2021-03-23 08:49:43
date last changed
2024-07-12 13:09:59
@article{3b8c559a-e453-495d-b7ba-5321c9a15d1a,
  abstract     = {{<p>The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO<sub>2</sub> 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<sub>2</sub> 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 CO<sub>2</sub> reduction. As a result, the product generation rate of Au<sub>SA</sub>/Cd<sub>1−x</sub>S manifests a remarkable at least 113-fold enhancement compared with pristine Cd<sub>1−x</sub>S.</p>}},
  author       = {{Cao, Yuehan and Guo, Lan and Dan, Meng and Doronkin, Dmitry E. and Han, Chunqiu and Rao, Zhiqiang and Liu, Yang and Meng, Jie and Huang, Zeai and Zheng, Kaibo and Chen, Peng and Dong, Fan and Zhou, Ying}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Modulating electron density of vacancy site by single Au atom for effective CO<sub>2</sub> photoreduction}},
  url          = {{http://dx.doi.org/10.1038/s41467-021-21925-7}},
  doi          = {{10.1038/s41467-021-21925-7}},
  volume       = {{12}},
  year         = {{2021}},
}