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

Tang, Yan1,2,3,4,5; Asokan, Chithra6; Xu, Mingjie7; Graham, George W.7,8; Pan, Xiaoqing7,9,10; Christopher, Phillip6; Li, Jun1,2,11; Sautet, Philippe3,4,5

2019-10-03

10.1038/s41467-019-12461-6

Nature Communications   影响因子和分区

2041-1723

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 TiO2 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.

SCI

英语

ESI高被引 ; NI期刊 ; ESI高被引 ; ESI高被引 ; ESI高被引

通讯

National Science Foundation Major Research Instrumentation Program[CHE-1338173]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000488774200004

NATURE PUBLISHING GROUP

Web of Science

1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
2.Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China
3.Univ Calif Los Angeles, Dept Chem & Biomol Engn, Los Angeles, CA 90095 USA
4.Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA
5.Univ Calif Los Angeles, Calif NanoSyst Inst, Los Angeles, CA 90095 USA
6.Univ Calif Santa Barbara, Dept Chem Engn, Santa Barbara, CA 93106 USA
7.Univ Calif Irvine, Dept Mat Sci & Engn, Irvine, CA 92697 USA
8.Univ Michigan, Dept Mat Sci & Engn, Ann Arbor, MI 48109 USA
9.Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA
10.Univ Calif Irvine, IMRI, Irvine, CA 92697 USA
11.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Tang, Yan,Asokan, Chithra,Xu, Mingjie,et al. Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site[J]. Nature Communications,2019,10.

Tang, Yan.,Asokan, Chithra.,Xu, Mingjie.,Graham, George W..,Pan, Xiaoqing.,...&Sautet, Philippe.(2019).Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site.Nature Communications,10.

Tang, Yan,et al."Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site".Nature Communications 10(2019).