Zhang, Wuyong ; Zhan, Shaoqi ; Xiao, Jie ; Petit, Tristan ; Schlesiger, Christopher ; Mellin, Maximilian ; Hofmann, Jan P. ; Heil, Tobias ; Müller, Riccarda ; Leopold, Kerstin ; Oschatz, Martin (2023)
Coordinative stabilization of single bismuth sites in a carbon–nitrogen matrix to generate atom‐efficient catalysts for electrochemical nitrate reduction to ammonia.
In: Advanced Science, 10 (28)
doi: 10.1002/advs.202302623
Artikel, Bibliographie
Dies ist die neueste Version dieses Eintrags.
Kurzbeschreibung (Abstract)
Electrochemical nitrate reduction to ammonia powered by renewable electricity is not only a promising alternative to the established energy‐intense and non‐ecofriendly Haber–Bosch reaction for ammonia generation but also a future contributor to the ever‐more important denitrification schemes. Nevertheless, this reaction is still impeded by the lack of understanding for the underlying reaction mechanism on the molecular scale which is necessary for the rational design of active, selective, and stable electrocatalysts. Herein, a novel single‐site bismuth catalyst (Bi‐N‐C) for nitrate electroreduction is reported to produce ammonia with maximum Faradaic efficiency of 88.7% and at a high rate of 1.38 mg h⁻¹ mgcat⁻¹ at −0.35 V versus reversible hydrogen electrode (RHE). The active center (described as BiN₂C₂) is uncovered by detailed structural analysis. Coupled density functional theory calculations are applied to analyze the reaction mechanism and potential rate‐limiting steps for nitrate reduction based on the BiN₂C₂ model. The findings highlight the importance of model catalysts to utilize the potential of nitrate reduction as a new‐generation nitrogen‐management technology based on the construction of efficient active sites.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2023 |
| Autor(en): | Zhang, Wuyong ; Zhan, Shaoqi ; Xiao, Jie ; Petit, Tristan ; Schlesiger, Christopher ; Mellin, Maximilian ; Hofmann, Jan P. ; Heil, Tobias ; Müller, Riccarda ; Leopold, Kerstin ; Oschatz, Martin |
| Art des Eintrags: | Bibliographie |
| Titel: | Coordinative stabilization of single bismuth sites in a carbon–nitrogen matrix to generate atom‐efficient catalysts for electrochemical nitrate reduction to ammonia |
| Sprache: | Englisch |
| Publikationsjahr: | 2023 |
| Ort: | Weinheim |
| Verlag: | Wiley-VCH |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Advanced Science |
| Jahrgang/Volume einer Zeitschrift: | 10 |
| (Heft-)Nummer: | 28 |
| Kollation: | 9 Seiten |
| DOI: | 10.1002/advs.202302623 |
| Zugehörige Links: | |
| Kurzbeschreibung (Abstract): | Electrochemical nitrate reduction to ammonia powered by renewable electricity is not only a promising alternative to the established energy‐intense and non‐ecofriendly Haber–Bosch reaction for ammonia generation but also a future contributor to the ever‐more important denitrification schemes. Nevertheless, this reaction is still impeded by the lack of understanding for the underlying reaction mechanism on the molecular scale which is necessary for the rational design of active, selective, and stable electrocatalysts. Herein, a novel single‐site bismuth catalyst (Bi‐N‐C) for nitrate electroreduction is reported to produce ammonia with maximum Faradaic efficiency of 88.7% and at a high rate of 1.38 mg h⁻¹ mgcat⁻¹ at −0.35 V versus reversible hydrogen electrode (RHE). The active center (described as BiN₂C₂) is uncovered by detailed structural analysis. Coupled density functional theory calculations are applied to analyze the reaction mechanism and potential rate‐limiting steps for nitrate reduction based on the BiN₂C₂ model. The findings highlight the importance of model catalysts to utilize the potential of nitrate reduction as a new‐generation nitrogen‐management technology based on the construction of efficient active sites. |
| Freie Schlagworte: | ammonia production, electrocatalysis, nitrate reduction reaction, single‐site catalysts |
| ID-Nummer: | Artikel-ID: 2302623 |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 600 Technik, Medizin, angewandte Wissenschaften > 660 Technische Chemie |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Oberflächenforschung |
| Hinterlegungsdatum: | 12 Feb 2024 07:50 |
| Letzte Änderung: | 12 Feb 2024 10:24 |
| PPN: | 515505447 |
| Zugehörige Links: | |
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| Suche nach Titel in: | TUfind oder in Google |
Verfügbare Versionen dieses Eintrags
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Coordinative Stabilization of Single Bismuth Sites in a Carbon–Nitrogen Matrix to Generate Atom‐Efficient Catalysts for Electrochemical Nitrate Reduction to Ammonia. (deposited 09 Feb 2024 14:09)
- Coordinative stabilization of single bismuth sites in a carbon–nitrogen matrix to generate atom‐efficient catalysts for electrochemical nitrate reduction to ammonia. (deposited 12 Feb 2024 07:50) [Gegenwärtig angezeigt]
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