Zheng, J, Wu, S, Lu, L 
ORCID: https://orcid.org/0000-0001-5722-0504, Huang, C, Ho, P-L, Kirkland, A, Sudmeier, T ORCID: https://orcid.org/0000-0002-0153-5387, Arrigo, R ORCID: https://orcid.org/0000-0002-2877-8733, Gianolio, D and Edman Tsang, SC ORCID: https://orcid.org/0000-0002-8796-3146
2021,
'Structural insight into [Fe–S2–Mo] motif in electrochemical reduction of N2 over Fe1-supported molecular MoS2'
, Chemical Science, 12 (2)
, pp. 688-695.
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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.
| Item Type: | Article |
|---|---|
| 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 |
| Schools: | Schools > School of Computing, Science and Engineering |
| Journal or Publication Title: | Chemical Science |
| Publisher: | Royal Society of Chemistry (RSC) |
| ISSN: | 2041-6520 |
| Related URLs: | |
| Funders: | Engineering and Physical Sciences Research Council (EPSRC) |
| SWORD Depositor: | Publications Router |
| Depositing User: | Publications Router |
| Date Deposited: | 23 Nov 2020 09:59 |
| Last Modified: | 01 Feb 2021 09:00 |
| URI: | http://usir.salford.ac.uk/id/eprint/58890 |
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