Structural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2
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 electroc...
| Main Authors: | , , , , , , , , , |
|---|---|
| Format: | Journal article |
| Language: | English |
| Published: |
Royal Society of Chemistry
2020
|
| _version_ | 1797104782639366144 |
|---|---|
| author | Zheng, J Wu, S Lu, L Huang, C Ho, P-L Kirkland, A Sudmeier, T Arrigo, R Gianolio, D Tsang, SCE |
| author_facet | Zheng, J Wu, S Lu, L Huang, C Ho, P-L Kirkland, A Sudmeier, T Arrigo, R Gianolio, D Tsang, SCE |
| author_sort | Zheng, J |
| collection | OXFORD |
| description | 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. |
| first_indexed | 2024-03-07T06:38:22Z |
| format | Journal article |
| id | oxford-uuid:f86f3415-d435-4f66-9b9b-30ec37d3aed8 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T06:38:22Z |
| publishDate | 2020 |
| publisher | Royal Society of Chemistry |
| record_format | dspace |
| spelling | oxford-uuid:f86f3415-d435-4f66-9b9b-30ec37d3aed82022-03-27T12:50:13ZStructural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:f86f3415-d435-4f66-9b9b-30ec37d3aed8EnglishSymplectic ElementsRoyal Society of Chemistry2020Zheng, JWu, SLu, LHuang, CHo, P-LKirkland, ASudmeier, TArrigo, RGianolio, DTsang, SCEThe 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. |
| spellingShingle | Zheng, J Wu, S Lu, L Huang, C Ho, P-L Kirkland, A Sudmeier, T Arrigo, R Gianolio, D Tsang, SCE Structural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2 |
| title | Structural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2 |
| title_full | Structural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2 |
| title_fullStr | Structural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2 |
| title_full_unstemmed | Structural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2 |
| title_short | Structural insight into [Fe-S-2-Mo] motif in electrochemical reduction of N-2 over Fe-1-supported molecular MoS2 |
| title_sort | structural insight into fe s 2 mo motif in electrochemical reduction of n 2 over fe 1 supported molecular mos2 |
| work_keys_str_mv | AT zhengj structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT wus structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT lul structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT huangc structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT hopl structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT kirklanda structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT sudmeiert structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT arrigor structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT gianoliod structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 AT tsangsce structuralinsightintofes2momotifinelectrochemicalreductionofn2overfe1supportedmolecularmos2 |