Biomimetic Design of a Dynamic M-O-V Pyramid Electron Bridge for Enhanced Nitrogen Electroreduction
Electrochemical nitrogen reduction reaction (eNRR) offers a sustainable route for ammonia synthesis; however, current electrocatalysts are limited in achieving optimal performance within narrow potential windows. Herein, inspired by the heliotropism of sunflowers, we present a biomimetic design of Ru-VOH electrocatalyst, featuring a dynamic Ru-O-V pyramid electron bridge for eNRR within a wide potential range. In situ spectroscopy and theoretical investigations unravel the fact that the electrons are donated from Ru to V at lower overpotentials and retrieved at higher overpotentials, maintaining a delicate balance between N2 activation and proton hydrogenation. Moreover, N2 adsorption and activation were found to be enhanced by the Ru-O-V moiety. The catalyst showcases an outstanding Faradaic efficiency of 51.48% at -0.2 V (vs RHE) with an NH3 yield rate exceeding 115 μg h-1 mg-1 across the range of -0.2 to -0.4 V (vs RHE), along with impressive durability of over 100 cycles. This dynamic M-O-V pyramid electron bridge is also applicable to other metals (M = Pt, Rh, and Pd).
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:146 |
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| Enthalten in: |
Journal of the American Chemical Society - 146(2024), 11 vom: 20. März, Seite 7752-7762 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Sun, Yuntong [VerfasserIn] |
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| Anmerkungen: |
Date Revised 20.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1021/jacs.3c14816 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM369369394 |
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| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Electrochemical nitrogen reduction reaction (eNRR) offers a sustainable route for ammonia synthesis; however, current electrocatalysts are limited in achieving optimal performance within narrow potential windows. Herein, inspired by the heliotropism of sunflowers, we present a biomimetic design of Ru-VOH electrocatalyst, featuring a dynamic Ru-O-V pyramid electron bridge for eNRR within a wide potential range. In situ spectroscopy and theoretical investigations unravel the fact that the electrons are donated from Ru to V at lower overpotentials and retrieved at higher overpotentials, maintaining a delicate balance between N2 activation and proton hydrogenation. Moreover, N2 adsorption and activation were found to be enhanced by the Ru-O-V moiety. The catalyst showcases an outstanding Faradaic efficiency of 51.48% at -0.2 V (vs RHE) with an NH3 yield rate exceeding 115 μg h-1 mg-1 across the range of -0.2 to -0.4 V (vs RHE), along with impressive durability of over 100 cycles. This dynamic M-O-V pyramid electron bridge is also applicable to other metals (M = Pt, Rh, and Pd) | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Li, Xuheng |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Zhiqi |e verfasserin |4 aut | |
| 700 | 1 | |a Jiang, Lili |e verfasserin |4 aut | |
| 700 | 1 | |a Mei, Bingbao |e verfasserin |4 aut | |
| 700 | 1 | |a Fan, Wenjun |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Junjie |e verfasserin |4 aut | |
| 700 | 1 | |a Zhu, Junwu |e verfasserin |4 aut | |
| 700 | 1 | |a Lee, Jong-Min |e verfasserin |4 aut | |
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