Synergizing Fe2O3 Nanoparticles on Single Atom Fe-N-C for Nitrate Reduction to Ammonia at Industrial Current Densities
© 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH..
The electrochemical reduction of nitrates (NO3 -) enables a pathway for the carbon neutral synthesis of ammonia (NH3), via the nitrate reduction reaction (NO3RR), which has been demonstrated at high selectivity. However, to make NH3 synthesis cost-competitive with current technologies, high NH3 partial current densities (jNH3) must be achieved to reduce the levelized cost of NH3. Here, the high NO3RR activity of Fe-based materials is leveraged to synthesize a novel active particle-active support system with Fe2O3 nanoparticles supported on atomically dispersed Fe-N-C. The optimized 3×Fe2O3/Fe-N-C catalyst demonstrates an ultrahigh NO3RR activity, reaching a maximum jNH3 of 1.95 A cm-2 at a Faradaic efficiency (FE) for NH3 of 100% and an NH3 yield rate over 9 mmol hr-1 cm-2. Operando XANES and post-mortem XPS reveal the importance of a pre-reduction activation step, reducing the surface Fe2O3 (Fe3+) to highly active Fe0 sites, which are maintained during electrolysis. Durability studies demonstrate the robustness of both the Fe2O3 particles and Fe-Nx sites at highly cathodic potentials, maintaining a current of -1.3 A cm-2 over 24 hours. This work exhibits an effective and durable active particle-active support system enhancing the performance of the NO3RR, enabling industrially relevant current densities and near 100% selectivity.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - year:2024 |
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| Enthalten in: |
Advanced materials (Deerfield Beach, Fla.) - (2024) vom: 15. Apr., Seite e2401133 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Murphy, Eamonn [VerfasserIn] |
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| Links: |
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| Themen: |
Active support |
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| Anmerkungen: |
Date Revised 28.04.2024 published: Print-Electronic Citation Status Publisher |
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| doi: |
10.1002/adma.202401133 |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM371092418 |
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| 245 | 1 | 0 | |a Synergizing Fe2O3 Nanoparticles on Single Atom Fe-N-C for Nitrate Reduction to Ammonia at Industrial Current Densities |
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| 520 | |a © 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH. | ||
| 520 | |a The electrochemical reduction of nitrates (NO3 -) enables a pathway for the carbon neutral synthesis of ammonia (NH3), via the nitrate reduction reaction (NO3RR), which has been demonstrated at high selectivity. However, to make NH3 synthesis cost-competitive with current technologies, high NH3 partial current densities (jNH3) must be achieved to reduce the levelized cost of NH3. Here, the high NO3RR activity of Fe-based materials is leveraged to synthesize a novel active particle-active support system with Fe2O3 nanoparticles supported on atomically dispersed Fe-N-C. The optimized 3×Fe2O3/Fe-N-C catalyst demonstrates an ultrahigh NO3RR activity, reaching a maximum jNH3 of 1.95 A cm-2 at a Faradaic efficiency (FE) for NH3 of 100% and an NH3 yield rate over 9 mmol hr-1 cm-2. Operando XANES and post-mortem XPS reveal the importance of a pre-reduction activation step, reducing the surface Fe2O3 (Fe3+) to highly active Fe0 sites, which are maintained during electrolysis. Durability studies demonstrate the robustness of both the Fe2O3 particles and Fe-Nx sites at highly cathodic potentials, maintaining a current of -1.3 A cm-2 over 24 hours. This work exhibits an effective and durable active particle-active support system enhancing the performance of the NO3RR, enabling industrially relevant current densities and near 100% selectivity | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a active support | |
| 650 | 4 | |a alkaline | |
| 650 | 4 | |a ammonia | |
| 650 | 4 | |a in situ XAS | |
| 650 | 4 | |a iron oxide | |
| 650 | 4 | |a nitrate reduction | |
| 650 | 4 | |a nitrite reduction | |
| 650 | 4 | |a single atom catalysts | |
| 700 | 1 | |a Sun, Baiyu |e verfasserin |4 aut | |
| 700 | 1 | |a Rüscher, Martina |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Yuanchao |e verfasserin |4 aut | |
| 700 | 1 | |a Zang, Wenjie |e verfasserin |4 aut | |
| 700 | 1 | |a Guo, Shengyuan |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Yu-Han |e verfasserin |4 aut | |
| 700 | 1 | |a Hejral, Uta |e verfasserin |4 aut | |
| 700 | 1 | |a Huang, Ying |e verfasserin |4 aut | |
| 700 | 1 | |a Ly, Alvin |e verfasserin |4 aut | |
| 700 | 1 | |a Zenyuk, Iryna V |e verfasserin |4 aut | |
| 700 | 1 | |a Pan, Xiaoqing |e verfasserin |4 aut | |
| 700 | 1 | |a Timoshenko, Janis |e verfasserin |4 aut | |
| 700 | 1 | |a Cuenya, Beatriz Roldán |e verfasserin |4 aut | |
| 700 | 1 | |a Spoerke, Erik D |e verfasserin |4 aut | |
| 700 | 1 | |a Atanassov, Plamen |e verfasserin |4 aut | |
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