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Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate

Pd metal and Pd-based alloys are ideal catalysts that allow for the electrochemical conversion of CO(2) to HCOO(−) at almost zero-overpotential with high selectivity, but catalyst degradation caused by concurrent CO poisoning limits their practical implementation. Here, we demonstrate that cyclic tw...

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Autores principales: Lee, Chan Woo, Cho, Nam Heon, Nam, Ki Tae, Hwang, Yun Jeong, Min, Byoung Koun
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6718411/
https://www.ncbi.nlm.nih.gov/pubmed/31477719
http://dx.doi.org/10.1038/s41467-019-11903-5
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author Lee, Chan Woo
Cho, Nam Heon
Nam, Ki Tae
Hwang, Yun Jeong
Min, Byoung Koun
author_facet Lee, Chan Woo
Cho, Nam Heon
Nam, Ki Tae
Hwang, Yun Jeong
Min, Byoung Koun
author_sort Lee, Chan Woo
collection PubMed
description Pd metal and Pd-based alloys are ideal catalysts that allow for the electrochemical conversion of CO(2) to HCOO(−) at almost zero-overpotential with high selectivity, but catalyst degradation caused by concurrent CO poisoning limits their practical implementation. Here, we demonstrate that cyclic two-step electrolysis, by applying the reduction and oxidation potentials alternately, achieves 100% current density stability and 97.8% selectivity toward HCOO(−) production for at least 45 h. The key idea for achieving the reliability is based on the selective removal of CO by controlling the parameters during the oxidation step, which utilizes the different reversibility of HCOO(−) and CO production reactions. Furthermore, it is found that potentiostatic electrolysis causes CO adsorption and subsequent dehydridation, which in turn lowers HCOO(−) selectivity. Our work provides a system-level strategy for solving the poisoning issue that is inevitable in many electrocatalytic reactions.
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spelling pubmed-67184112019-09-04 Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate Lee, Chan Woo Cho, Nam Heon Nam, Ki Tae Hwang, Yun Jeong Min, Byoung Koun Nat Commun Article Pd metal and Pd-based alloys are ideal catalysts that allow for the electrochemical conversion of CO(2) to HCOO(−) at almost zero-overpotential with high selectivity, but catalyst degradation caused by concurrent CO poisoning limits their practical implementation. Here, we demonstrate that cyclic two-step electrolysis, by applying the reduction and oxidation potentials alternately, achieves 100% current density stability and 97.8% selectivity toward HCOO(−) production for at least 45 h. The key idea for achieving the reliability is based on the selective removal of CO by controlling the parameters during the oxidation step, which utilizes the different reversibility of HCOO(−) and CO production reactions. Furthermore, it is found that potentiostatic electrolysis causes CO adsorption and subsequent dehydridation, which in turn lowers HCOO(−) selectivity. Our work provides a system-level strategy for solving the poisoning issue that is inevitable in many electrocatalytic reactions. Nature Publishing Group UK 2019-09-02 /pmc/articles/PMC6718411/ /pubmed/31477719 http://dx.doi.org/10.1038/s41467-019-11903-5 Text en © The Author(s) 2019 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/.
spellingShingle Article
Lee, Chan Woo
Cho, Nam Heon
Nam, Ki Tae
Hwang, Yun Jeong
Min, Byoung Koun
Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate
title Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate
title_full Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate
title_fullStr Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate
title_full_unstemmed Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate
title_short Cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate
title_sort cyclic two-step electrolysis for stable electrochemical conversion of carbon dioxide to formate
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6718411/
https://www.ncbi.nlm.nih.gov/pubmed/31477719
http://dx.doi.org/10.1038/s41467-019-11903-5
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