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Single-Metal-Atom Dopants Increase the Lewis Acidity of Metal Oxides and Promote Nitrogen Fixation

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Title
Single-Metal-Atom Dopants Increase the Lewis Acidity of Metal Oxides and Promote Nitrogen Fixation
Author(s)
Jinsun Lee; Ashwani Kumar; Kim, Min Gyu; Taehun Yang; Xiaodong Shao; Xinghui Liu; Yang Liu; Yeseul Hong; Amol R. Jadhav; Mengfang Liang; Ngoc Quang Tran; Hyoyoung Lee
Publication Date
2021-12-10
Journal
ACS Energy Letters, v.6, no.12, pp.4299 - 4308
Publisher
American Chemical Society
Abstract
© 2021 American Chemical Society.Exploring Earth-abundant metal oxides for ambient N2 (Lewis base) reduction to value-added NH3, an essential commodity for modern industries, has extreme significance. However, due to their insufficient Lewis acidity and unfavorable electronic parameters, resulting in poor N2 adsorption, instability of key N intermediates (NNH*/NNH2*/N*), and preference for hydrogen evolution, the NH3 selectivity and yield rate with metal oxides are far from satisfactory. Herein, theoretical predictions reveal that tuning the electronic structure of defective Co3O4 (Co3O4-x) via a single-Ru-atom dopant can cooperatively enhance the N2 adsorption, driven by strong Ru4d-N2p orbital coupling, and stabilize the key N-intermediates, further suppressing the H∗ dimerization and significantly boosting the NH3 selectivity. Motivated by DFT predictions, we introduced optimal single-Ru-atom dopants to maximize the Lewis acidity of Co3O4 with in situ-generated oxygen defects (Ru1.4Co3O4-x), which exhibited an excellent N2-fixation activity with a high NH3 Faradaic efficiency (40.2%) and yield rate (39.4 μg/h/mgcat; 2.67 mg/h/mgRu) at 0 V (vs RHE), along with long-term stability and 2.5 times higher selectivity than pristine Co3O4-x, outperforming the state-of-the-art Ru/C.
URI
https://pr.ibs.re.kr/handle/8788114/10988
DOI
10.1021/acsenergylett.1c02136
ISSN
2380-8195
Appears in Collections:
Center for Integrated Nanostructure Physics(나노구조물리 연구단) > 1. Journal Papers (저널논문)
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