J Zheng
Structural insight into [Fe–S2–Mo] motif in electrochemical reduction of N2 over Fe1-supported molecular MoS2
Zheng, J; Wu, S; Lu, L; Huang, C; Ho, P-L; Kirkland, A; Sudmeier, T; Arrigo, R; Gianolio, D; Edman Tsang, SC
Authors
S Wu
L Lu
C Huang
P-L Ho
A Kirkland
T Sudmeier
Dr Rosa Arrigo R.Arrigo@salford.ac.uk
Reader
D Gianolio
SC Edman Tsang
Abstract
The catalytic synthesis of NH3 from the thermodynamically challenging N2 reduction reaction under mild conditions is currently a significant problem for scientists. Accordingly, herein, we report the development of a nitrogenase-inspired inorganic-based chalcogenide system for the efficient electrochemical conversion of N2 to NH3, which is comprised of the basic structure of [Fe–S2–Mo]. This material showed high activity of 8.7 mgNH3 mgFe−1 h−1 (24 μgNH3 cm−2 h−1) with an excellent faradaic efficiency of 27% for the conversion of N2 to NH3 in aqueous medium. It was demonstrated that the Fe1 single atom on [Fe–S2–Mo] under the optimal negative potential favors the reduction of N2 to NH3 over the competitive proton reduction to H2. Operando X-ray absorption and simulations combined with theoretical DFT calculations provided the first and important insights on the particular electron-mediating and catalytic roles of the [Fe–S2–Mo] motifs and Fe1, respectively, on this two-dimensional (2D) molecular layer slab.
Citation
Zheng, J., Wu, S., Lu, L., Huang, C., Ho, P., Kirkland, A., …Edman Tsang, S. (2021). Structural insight into [Fe–S2–Mo] motif in electrochemical reduction of N2 over Fe1-supported molecular MoS2. Chemical Science, 12(2), 688-695. https://doi.org/10.1039/d0sc04575f
Journal Article Type | Article |
---|---|
Acceptance Date | Oct 21, 2020 |
Online Publication Date | Nov 12, 2020 |
Publication Date | Jan 14, 2021 |
Deposit Date | Nov 23, 2020 |
Publicly Available Date | Nov 23, 2020 |
Journal | Chemical Science |
Print ISSN | 2041-6520 |
Electronic ISSN | 2041-6539 |
Publisher | Royal Society of Chemistry |
Volume | 12 |
Issue | 2 |
Pages | 688-695 |
DOI | https://doi.org/10.1039/d0sc04575f |
Publisher URL | https://doi.org/10.1039/D0SC04575F |
Related Public URLs | https://pubs.rsc.org/en/journals/journal/sc |
Additional Information | Additional Information : ** Article version: VoR ** From Crossref journal articles via Jisc Publications Router ** Licence for VoR version of this article starting on 12-11-2020: http://creativecommons.org/licenses/by-nc/3.0/ **Journal IDs: pissn 2041-6520; eissn 2041-6539 **History: published 2021 Funders : Engineering and Physical Sciences Research Council (EPSRC);Engineering and Physical Sciences Research Council Projects : DGE 102000 Grant Number: DGE 102000 |
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Publisher Licence URL
http://creativecommons.org/licenses/by-nc/3.0/
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