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Title: Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site

Abstract

Abstract Single-atom catalysts are widely investigated heterogeneous catalysts; however, the identification of the local environment of single atoms under experimental conditions, as well as operando characterization of their structural changes during catalytic reactions are still challenging. Here, the preferred local coordination of Rh single atoms is investigated on TiO 2 during calcination in O 2 , reduction in H 2 , CO adsorption, and reverse water gas shift (RWGS) reaction conditions. Theoretical and experimental studies clearly demonstrate that Rh single atoms adapt their local coordination and reactivity in response to various redox conditions. Single-atom catalysts hence do not have static local coordinations, but can switch from inactive to active structure under reaction conditions, hence explaining some conflicting literature accounts. The combination of approaches also elucidates the structure of the catalytic active site during reverse water gas shift. This insight on the real nature of the active site is key for the design of high-performance catalysts.

Authors:
; ; ; ; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); China Scholarship Council; National Science Foundation (NSF); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1619720
Alternate Identifier(s):
OSTI ID: 1595588
Grant/Contract Number:  
SC0012573
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 10 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English

Citation Formats

Tang, Yan, Asokan, Chithra, Xu, Mingjie, Graham, George W., Pan, Xiaoqing, Christopher, Phillip, Li, Jun, and Sautet, Philippe. Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site. United Kingdom: N. p., 2019. Web. doi:10.1038/s41467-019-12461-6.
Tang, Yan, Asokan, Chithra, Xu, Mingjie, Graham, George W., Pan, Xiaoqing, Christopher, Phillip, Li, Jun, & Sautet, Philippe. Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site. United Kingdom. doi:10.1038/s41467-019-12461-6.
Tang, Yan, Asokan, Chithra, Xu, Mingjie, Graham, George W., Pan, Xiaoqing, Christopher, Phillip, Li, Jun, and Sautet, Philippe. Thu . "Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site". United Kingdom. doi:10.1038/s41467-019-12461-6.
@article{osti_1619720,
title = {Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site},
author = {Tang, Yan and Asokan, Chithra and Xu, Mingjie and Graham, George W. and Pan, Xiaoqing and Christopher, Phillip and Li, Jun and Sautet, Philippe},
abstractNote = {Abstract Single-atom catalysts are widely investigated heterogeneous catalysts; however, the identification of the local environment of single atoms under experimental conditions, as well as operando characterization of their structural changes during catalytic reactions are still challenging. Here, the preferred local coordination of Rh single atoms is investigated on TiO 2 during calcination in O 2 , reduction in H 2 , CO adsorption, and reverse water gas shift (RWGS) reaction conditions. Theoretical and experimental studies clearly demonstrate that Rh single atoms adapt their local coordination and reactivity in response to various redox conditions. Single-atom catalysts hence do not have static local coordinations, but can switch from inactive to active structure under reaction conditions, hence explaining some conflicting literature accounts. The combination of approaches also elucidates the structure of the catalytic active site during reverse water gas shift. This insight on the real nature of the active site is key for the design of high-performance catalysts.},
doi = {10.1038/s41467-019-12461-6},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United Kingdom},
year = {2019},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1038/s41467-019-12461-6

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Cited by: 12 works
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