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Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst

Conversion into high-value-added organic nitrogen compounds through electrochemical C-N coupling reactions under ambient conditions is regarded as a sustainable development strategy to achieve carbon neutrality and high-value utilization of harmful substances. Herein, we report an electrochemical pr...

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Autores principales: Lan, Jiao, Wei, Zengxi, Lu, Ying-Rui, Chen, DeChao, Zhao, Shuangliang, Chan, Ting-Shan, Tan, Yongwen
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10198976/
https://www.ncbi.nlm.nih.gov/pubmed/37208321
http://dx.doi.org/10.1038/s41467-023-38603-5
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author Lan, Jiao
Wei, Zengxi
Lu, Ying-Rui
Chen, DeChao
Zhao, Shuangliang
Chan, Ting-Shan
Tan, Yongwen
author_facet Lan, Jiao
Wei, Zengxi
Lu, Ying-Rui
Chen, DeChao
Zhao, Shuangliang
Chan, Ting-Shan
Tan, Yongwen
author_sort Lan, Jiao
collection PubMed
description Conversion into high-value-added organic nitrogen compounds through electrochemical C-N coupling reactions under ambient conditions is regarded as a sustainable development strategy to achieve carbon neutrality and high-value utilization of harmful substances. Herein, we report an electrochemical process for selective synthesis of high-valued formamide from carbon monoxide and nitrite with a Ru(1)Cu single-atom alloy under ambient conditions, which achieves a high formamide selectivity with Faradaic efficiency of 45.65 ± 0.76% at −0.5 V vs. RHE. In situ X-ray absorption spectroscopy, coupled with in situ Raman spectroscopy and density functional theory calculations results reveal that the adjacent Ru-Cu dual active sites can spontaneously couple *CO and *NH(2) intermediates to realize a critical C-N coupling reaction, enabling high-performance electrosynthesis of formamide. This work offers insight into the high-value formamide electrocatalysis through coupling CO and NO(2)(−) under ambient conditions, paving the way for the synthesis of more-sustainable and high-value chemical products.
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spelling pubmed-101989762023-05-21 Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst Lan, Jiao Wei, Zengxi Lu, Ying-Rui Chen, DeChao Zhao, Shuangliang Chan, Ting-Shan Tan, Yongwen Nat Commun Article Conversion into high-value-added organic nitrogen compounds through electrochemical C-N coupling reactions under ambient conditions is regarded as a sustainable development strategy to achieve carbon neutrality and high-value utilization of harmful substances. Herein, we report an electrochemical process for selective synthesis of high-valued formamide from carbon monoxide and nitrite with a Ru(1)Cu single-atom alloy under ambient conditions, which achieves a high formamide selectivity with Faradaic efficiency of 45.65 ± 0.76% at −0.5 V vs. RHE. In situ X-ray absorption spectroscopy, coupled with in situ Raman spectroscopy and density functional theory calculations results reveal that the adjacent Ru-Cu dual active sites can spontaneously couple *CO and *NH(2) intermediates to realize a critical C-N coupling reaction, enabling high-performance electrosynthesis of formamide. This work offers insight into the high-value formamide electrocatalysis through coupling CO and NO(2)(−) under ambient conditions, paving the way for the synthesis of more-sustainable and high-value chemical products. Nature Publishing Group UK 2023-05-19 /pmc/articles/PMC10198976/ /pubmed/37208321 http://dx.doi.org/10.1038/s41467-023-38603-5 Text en © The Author(s) 2023 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
Lan, Jiao
Wei, Zengxi
Lu, Ying-Rui
Chen, DeChao
Zhao, Shuangliang
Chan, Ting-Shan
Tan, Yongwen
Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst
title Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst
title_full Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst
title_fullStr Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst
title_full_unstemmed Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst
title_short Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst
title_sort efficient electrosynthesis of formamide from carbon monoxide and nitrite on a ru-dispersed cu nanocluster catalyst
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10198976/
https://www.ncbi.nlm.nih.gov/pubmed/37208321
http://dx.doi.org/10.1038/s41467-023-38603-5
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