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Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling

Electroreduction of carbon dioxide (CO(2)) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically lo...

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Autores principales: Wang, Pengtang, Yang, Hao, Tang, Cheng, Wu, Yu, Zheng, Yao, Cheng, Tao, Davey, Kenneth, Huang, Xiaoqing, Qiao, Shi-Zhang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9243136/
https://www.ncbi.nlm.nih.gov/pubmed/35768462
http://dx.doi.org/10.1038/s41467-022-31427-9
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author Wang, Pengtang
Yang, Hao
Tang, Cheng
Wu, Yu
Zheng, Yao
Cheng, Tao
Davey, Kenneth
Huang, Xiaoqing
Qiao, Shi-Zhang
author_facet Wang, Pengtang
Yang, Hao
Tang, Cheng
Wu, Yu
Zheng, Yao
Cheng, Tao
Davey, Kenneth
Huang, Xiaoqing
Qiao, Shi-Zhang
author_sort Wang, Pengtang
collection PubMed
description Electroreduction of carbon dioxide (CO(2)) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver–modified copper–oxide catalyst (dCu(2)O/Ag(2.3%)) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO(2)–to–ethanol conversion under high current operation with partial current density of 326.4 mA cm(−2) at −0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu–based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the (*)CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C–C coupling for stablization of EtOH intermediates.
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spelling pubmed-92431362022-07-01 Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling Wang, Pengtang Yang, Hao Tang, Cheng Wu, Yu Zheng, Yao Cheng, Tao Davey, Kenneth Huang, Xiaoqing Qiao, Shi-Zhang Nat Commun Article Electroreduction of carbon dioxide (CO(2)) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver–modified copper–oxide catalyst (dCu(2)O/Ag(2.3%)) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO(2)–to–ethanol conversion under high current operation with partial current density of 326.4 mA cm(−2) at −0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu–based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the (*)CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C–C coupling for stablization of EtOH intermediates. Nature Publishing Group UK 2022-06-29 /pmc/articles/PMC9243136/ /pubmed/35768462 http://dx.doi.org/10.1038/s41467-022-31427-9 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
Wang, Pengtang
Yang, Hao
Tang, Cheng
Wu, Yu
Zheng, Yao
Cheng, Tao
Davey, Kenneth
Huang, Xiaoqing
Qiao, Shi-Zhang
Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling
title Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling
title_full Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling
title_fullStr Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling
title_full_unstemmed Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling
title_short Boosting electrocatalytic CO(2)–to–ethanol production via asymmetric C–C coupling
title_sort boosting electrocatalytic co(2)–to–ethanol production via asymmetric c–c coupling
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9243136/
https://www.ncbi.nlm.nih.gov/pubmed/35768462
http://dx.doi.org/10.1038/s41467-022-31427-9
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