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On the importance of the electric double layer structure in aqueous electrocatalysis
To design electrochemical interfaces for efficient electric-chemical energy interconversion, it is critical to reveal the electric double layer (EDL) structure and relate it with electrochemical activity; nonetheless, this has been a long-standing challenge. Of particular, no molecular-level theorie...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8748683/ https://www.ncbi.nlm.nih.gov/pubmed/35013347 http://dx.doi.org/10.1038/s41467-021-27909-x |
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author | Shin, Seung-Jae Kim, Dong Hyun Bae, Geunsu Ringe, Stefan Choi, Hansol Lim, Hyung-Kyu Choi, Chang Hyuck Kim, Hyungjun |
author_facet | Shin, Seung-Jae Kim, Dong Hyun Bae, Geunsu Ringe, Stefan Choi, Hansol Lim, Hyung-Kyu Choi, Chang Hyuck Kim, Hyungjun |
author_sort | Shin, Seung-Jae |
collection | PubMed |
description | To design electrochemical interfaces for efficient electric-chemical energy interconversion, it is critical to reveal the electric double layer (EDL) structure and relate it with electrochemical activity; nonetheless, this has been a long-standing challenge. Of particular, no molecular-level theories have fully explained the characteristic two peaks arising in the potential-dependence of the EDL capacitance, which is sensitively dependent on the EDL structure. We herein demonstrate that our first-principles-based molecular simulation reproduces the experimental capacitance peaks. The origin of two peaks emerging at anodic and cathodic potentials is unveiled to be an electrosorption of ions and a structural phase transition, respectively. We further find a cation complexation gradually modifies the EDL structure and the field strength, which linearly scales the carbon dioxide reduction activity. This study deciphers the complex structural response of the EDL and highlights its catalytic importance, which bridges the mechanistic gap between the EDL structure and electrocatalysis. |
format | Online Article Text |
id | pubmed-8748683 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-87486832022-01-20 On the importance of the electric double layer structure in aqueous electrocatalysis Shin, Seung-Jae Kim, Dong Hyun Bae, Geunsu Ringe, Stefan Choi, Hansol Lim, Hyung-Kyu Choi, Chang Hyuck Kim, Hyungjun Nat Commun Article To design electrochemical interfaces for efficient electric-chemical energy interconversion, it is critical to reveal the electric double layer (EDL) structure and relate it with electrochemical activity; nonetheless, this has been a long-standing challenge. Of particular, no molecular-level theories have fully explained the characteristic two peaks arising in the potential-dependence of the EDL capacitance, which is sensitively dependent on the EDL structure. We herein demonstrate that our first-principles-based molecular simulation reproduces the experimental capacitance peaks. The origin of two peaks emerging at anodic and cathodic potentials is unveiled to be an electrosorption of ions and a structural phase transition, respectively. We further find a cation complexation gradually modifies the EDL structure and the field strength, which linearly scales the carbon dioxide reduction activity. This study deciphers the complex structural response of the EDL and highlights its catalytic importance, which bridges the mechanistic gap between the EDL structure and electrocatalysis. Nature Publishing Group UK 2022-01-10 /pmc/articles/PMC8748683/ /pubmed/35013347 http://dx.doi.org/10.1038/s41467-021-27909-x 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 Shin, Seung-Jae Kim, Dong Hyun Bae, Geunsu Ringe, Stefan Choi, Hansol Lim, Hyung-Kyu Choi, Chang Hyuck Kim, Hyungjun On the importance of the electric double layer structure in aqueous electrocatalysis |
title | On the importance of the electric double layer structure in aqueous electrocatalysis |
title_full | On the importance of the electric double layer structure in aqueous electrocatalysis |
title_fullStr | On the importance of the electric double layer structure in aqueous electrocatalysis |
title_full_unstemmed | On the importance of the electric double layer structure in aqueous electrocatalysis |
title_short | On the importance of the electric double layer structure in aqueous electrocatalysis |
title_sort | on the importance of the electric double layer structure in aqueous electrocatalysis |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8748683/ https://www.ncbi.nlm.nih.gov/pubmed/35013347 http://dx.doi.org/10.1038/s41467-021-27909-x |
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