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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

Zhang, Wuyong ; Zhan, Shaoqi ; Xiao, Jie ; Petit, Tristan ; Schlesiger, Christopher ; Mellin, Maximilian ; Hofmann, Jan P. ; Heil, Tobias ; Müller, Riccarda ; Leopold, Kerstin ; Oschatz, Martin (2024)
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, 2023, 10 (28)
doi: 10.26083/tuprints-00024666
Article, Secondary publication, Publisher's Version

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Item Type: Article
Type of entry: Secondary publication
Title: Coordinative Stabilization of Single Bismuth Sites in a Carbon–Nitrogen Matrix to Generate Atom‐Efficient Catalysts for Electrochemical Nitrate Reduction to Ammonia
Language: English
Date: 9 February 2024
Place of Publication: Darmstadt
Year of primary publication: 2023
Place of primary publication: Weinheim
Publisher: Wiley-VCH
Journal or Publication Title: Advanced Science
Volume of the journal: 10
Issue Number: 28
Collation: 9 Seiten
DOI: 10.26083/tuprints-00024666
Corresponding Links:
Origin: Secondary publication DeepGreen
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.

Uncontrolled Keywords: ammonia production, electrocatalysis, nitrate reduction reaction, single‐site catalysts
Identification Number: Artikel-ID: 2302623
Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-246663
Classification DDC: 600 Technology, medicine, applied sciences > 660 Chemical engineering
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Surface Science
Date Deposited: 09 Feb 2024 14:09
Last Modified: 09 Feb 2024 14:09
SWORD Depositor: Deep Green
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/24666
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