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Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature
The development of electrocatalysts capable of efficient reduction of nitrate (NO(3)(−)) to ammonia (NH(3)) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9780304/ https://www.ncbi.nlm.nih.gov/pubmed/36550156 http://dx.doi.org/10.1038/s41467-022-35533-6 |
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author | Fang, Jia-Yi Zheng, Qi-Zheng Lou, Yao-Yin Zhao, Kuang-Min Hu, Sheng-Nan Li, Guang Akdim, Ouardia Huang, Xiao-Yang Sun, Shi-Gang |
author_facet | Fang, Jia-Yi Zheng, Qi-Zheng Lou, Yao-Yin Zhao, Kuang-Min Hu, Sheng-Nan Li, Guang Akdim, Ouardia Huang, Xiao-Yang Sun, Shi-Gang |
author_sort | Fang, Jia-Yi |
collection | PubMed |
description | The development of electrocatalysts capable of efficient reduction of nitrate (NO(3)(−)) to ammonia (NH(3)) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO(2)(−) via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NO(x)(−) adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm(−2) at −0.2 V vs. Reversible Hydrogen Electrode. The NH(3) production rate reaches a high activity of 4.8 mmol cm(−2) h(−1) (960 mmol g(cat)(−1) h(−1)). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO(3)(−) to NH(3) via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO(3) led simultaneously to high NH(3) selectivity and yield. |
format | Online Article Text |
id | pubmed-9780304 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-97803042022-12-24 Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature Fang, Jia-Yi Zheng, Qi-Zheng Lou, Yao-Yin Zhao, Kuang-Min Hu, Sheng-Nan Li, Guang Akdim, Ouardia Huang, Xiao-Yang Sun, Shi-Gang Nat Commun Article The development of electrocatalysts capable of efficient reduction of nitrate (NO(3)(−)) to ammonia (NH(3)) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO(2)(−) via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NO(x)(−) adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm(−2) at −0.2 V vs. Reversible Hydrogen Electrode. The NH(3) production rate reaches a high activity of 4.8 mmol cm(−2) h(−1) (960 mmol g(cat)(−1) h(−1)). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO(3)(−) to NH(3) via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO(3) led simultaneously to high NH(3) selectivity and yield. Nature Publishing Group UK 2022-12-22 /pmc/articles/PMC9780304/ /pubmed/36550156 http://dx.doi.org/10.1038/s41467-022-35533-6 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Fang, Jia-Yi Zheng, Qi-Zheng Lou, Yao-Yin Zhao, Kuang-Min Hu, Sheng-Nan Li, Guang Akdim, Ouardia Huang, Xiao-Yang Sun, Shi-Gang Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature |
title | Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature |
title_full | Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature |
title_fullStr | Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature |
title_full_unstemmed | Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature |
title_short | Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature |
title_sort | ampere-level current density ammonia electrochemical synthesis using cuco nanosheets simulating nitrite reductase bifunctional nature |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9780304/ https://www.ncbi.nlm.nih.gov/pubmed/36550156 http://dx.doi.org/10.1038/s41467-022-35533-6 |
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