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

Cao, Yuehan (author)
Southwest Petroleum University
Guo, Lan (author)
Southwest Petroleum University
Dan, Meng (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Southwest Petroleum University
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Doronkin, Dmitry E. (author)
Karlsruhe Institute of Technology
Han, Chunqiu (author)
Southwest Petroleum University
Rao, Zhiqiang (author)
Southwest Petroleum University
Liu, Yang (author)
Southwest Petroleum University,Lund University
Meng, Jie (author)
Technical University of Denmark,Lund University
Huang, Zeai (author)
Southwest Petroleum University
Zheng, Kaibo (author)
Lund University,Lunds universitet,NanoLund: Centre for Nanoscience,Annan verksamhet, LTH,Lunds Tekniska Högskola,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Other operations, LTH,Faculty of Engineering, LTH,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH,Technical University of Denmark
Chen, Peng (author)
University of Electronic Science and Technology of China,Southwest Petroleum University
Dong, Fan (author)
University of Electronic Science and Technology of China
Zhou, Ying (author)
Southwest Petroleum University
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 (creator_code:org_t)
2021-03-15
2021
English.
In: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 12:1
Related links:
http://dx.doi.org/10... (free)
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https://www.nature.c...
https://lup.lub.lu.s...
https://doi.org/10.1...
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  • Journal article (peer-reviewed)
Abstract Subject headings
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  • 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.

Subject headings

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)

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