Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction
(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.
(Less)
- author
- organization
- publishing date
- 2021
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Nature Communications
- volume
- 12
- issue
- 1
- article number
- 1675
- publisher
- Nature Publishing Group
- external identifiers
-
- scopus:85102519602
- pmid:33723264
- 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
- 2024-09-06 16:27:20
@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}}, }