Identification of Cu(111) as Superior Active Sites for Electrocatalytic NO Reduction to NH3 with High Single-Pass Conversion Efficiency
© 2024 Wiley-VCH GmbH..
Opting for NO as an N source in electrocatalytic NH3 synthesis presents an intriguing approach to tackle energy and environmental challenges. However, blindly pursuing high NH3 synthesis rates and Faradaic efficiency (FE) while ignoring the NO conversion ratio could result in environmental problems. Herein, Cu nanosheets with exposed (111) surface is fabricated and exhibit a NO-to-NH3 yield rate of 371.89 μmol cm-2 h-1 (flow cell) and the highest FE of 93.19±1.99 % (H-type cell). The NO conversion ratio is increased to the current highest value of 63.74 % combined with the development of the flow cell. Additionally, Crystal Orbital Hamilton Population (COHP) clearly reveals that the "σ-π* acceptance-donation" is the essence of the interaction between the Cu and NO as also supported by operando attenuated total reflection infrared spectroscopy (ATR-IRAS) in observing the key intermediate of NO- . This work not only achieves a milestone NO conversion ratio for electrocatalytic NO-to-NH3 , but also proposes a new descriptor that utilizes orbital hybridization between molecules and metal centers to accurately identify the real active sites of catalysts.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:63 |
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| Enthalten in: |
Angewandte Chemie (International ed. in English) - 63(2024), 11 vom: 11. März, Seite e202319135 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Xiao, Lei [VerfasserIn] |
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| Links: |
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| Themen: |
Cu (111) |
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| Anmerkungen: |
Date Revised 04.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1002/anie.202319135 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM366763725 |
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| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a © 2024 Wiley-VCH GmbH. | ||
| 520 | |a Opting for NO as an N source in electrocatalytic NH3 synthesis presents an intriguing approach to tackle energy and environmental challenges. However, blindly pursuing high NH3 synthesis rates and Faradaic efficiency (FE) while ignoring the NO conversion ratio could result in environmental problems. Herein, Cu nanosheets with exposed (111) surface is fabricated and exhibit a NO-to-NH3 yield rate of 371.89 μmol cm-2 h-1 (flow cell) and the highest FE of 93.19±1.99 % (H-type cell). The NO conversion ratio is increased to the current highest value of 63.74 % combined with the development of the flow cell. Additionally, Crystal Orbital Hamilton Population (COHP) clearly reveals that the "σ-π* acceptance-donation" is the essence of the interaction between the Cu and NO as also supported by operando attenuated total reflection infrared spectroscopy (ATR-IRAS) in observing the key intermediate of NO- . This work not only achieves a milestone NO conversion ratio for electrocatalytic NO-to-NH3 , but also proposes a new descriptor that utilizes orbital hybridization between molecules and metal centers to accurately identify the real active sites of catalysts | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Cu (111) | |
| 650 | 4 | |a Electrocatalysis | |
| 650 | 4 | |a NH3 Synthesis | |
| 650 | 4 | |a NO Reduction | |
| 650 | 4 | |a Reaction Mechanism | |
| 700 | 1 | |a Mou, Shiyong |e verfasserin |4 aut | |
| 700 | 1 | |a Dai, Weidong |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Weiping |e verfasserin |4 aut | |
| 700 | 1 | |a Cheng, Qin |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Siyuan |e verfasserin |4 aut | |
| 700 | 1 | |a Dong, Fan |e verfasserin |4 aut | |
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