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

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.

SUBMITTER: Zheng J 

PROVIDER: S-EPMC8178972 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature

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Structural insight into [Fe-S<sub>2</sub>-Mo] motif in electrochemical reduction of N<sub>2</sub> over Fe<sub>1</sub>-supported molecular MoS<sub>2</sub>.

Zheng Jianwei J   Wu Simson S   Lu Lilin L   Huang Chen C   Ho Ping-Luen PL   Kirkland Angus A   Sudmeier Tim T   Arrigo Rosa R   Gianolio Diego D   Edman Tsang Shik Chi SC  

Chemical science 20201112 2

The catalytic synthesis of NH<sub>3</sub> from the thermodynamically challenging N<sub>2</sub> 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 N<sub>2</sub> to NH<sub>3</sub>, which is comprised of the basic structure of [Fe-S<sub>2</sub>-Mo]. This material showed high activity of 8.7 mg<sub>NH<sub  ...[more]

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