Structural insight into [Fe–S2–Mo] motif in electrochemical reduction of N2 over Fe1-supported molecular MoS2

Zheng, J, Wu, S, Lu, L ORCID:, Huang, C, Ho, P-L, Kirkland, A, Sudmeier, T ORCID:, Arrigo, R ORCID:, Gianolio, D and Edman Tsang, SC ORCID: 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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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: **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: 16 Feb 2022 06:18

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