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. / Cao, Yuehan; Guo, Lan; Dan, Meng; Doronkin, Dmitry E.; Han, Chunqiu; Rao, Zhiqiang; Liu, Yang; Meng, Jie; Huang, Zeai; Zheng, Kaibo; Chen, Peng; Dong, Fan; Zhou, Ying.

In: Nature Communications, Vol. 12, No. 1, 1675, 2021.

Research output: Contribution to journalArticle

Harvard

Cao, Y, Guo, L, Dan, M, Doronkin, DE, Han, C, Rao, Z, Liu, Y, Meng, J, Huang, Z, Zheng, K, Chen, P, Dong, F & Zhou, Y 2021, 'Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction', Nature Communications, vol. 12, no. 1, 1675. https://doi.org/10.1038/s41467-021-21925-7

APA

Cao, Y., Guo, L., Dan, M., Doronkin, D. E., Han, C., Rao, Z., Liu, Y., Meng, J., Huang, Z., Zheng, K., Chen, P., Dong, F., & Zhou, Y. (2021). Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction. Nature Communications, 12(1), [1675]. https://doi.org/10.1038/s41467-021-21925-7

CBE

Cao Y, Guo L, Dan M, Doronkin DE, Han C, Rao Z, Liu Y, Meng J, Huang Z, Zheng K, Chen P, Dong F, Zhou Y. 2021. Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction. Nature Communications. 12(1):Article 1675. https://doi.org/10.1038/s41467-021-21925-7

MLA

Vancouver

Author

Cao, Yuehan ; Guo, Lan ; Dan, Meng ; Doronkin, Dmitry E. ; Han, Chunqiu ; Rao, Zhiqiang ; Liu, Yang ; Meng, Jie ; Huang, Zeai ; Zheng, Kaibo ; Chen, Peng ; Dong, Fan ; Zhou, Ying. / Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction. In: Nature Communications. 2021 ; Vol. 12, No. 1.

RIS

TY - JOUR

T1 - Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

AU - Cao, Yuehan

AU - Guo, Lan

AU - Dan, Meng

AU - Doronkin, Dmitry E.

AU - Han, Chunqiu

AU - Rao, Zhiqiang

AU - Liu, Yang

AU - Meng, Jie

AU - Huang, Zeai

AU - Zheng, Kaibo

AU - Chen, Peng

AU - Dong, Fan

AU - Zhou, Ying

PY - 2021

Y1 - 2021

N2 - 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.

AB - 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.

U2 - 10.1038/s41467-021-21925-7

DO - 10.1038/s41467-021-21925-7

M3 - Article

C2 - 33723264

AN - SCOPUS:85102519602

VL - 12

JO - Nature Communications

JF - Nature Communications

SN - 2041-1723

IS - 1

M1 - 1675

ER -