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Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode
Electrochemical reduction of carbon dioxide is a clean and highly attractive strategy for the production of organic products. However, this is hindered severely by the high negative potential required to activate carbon dioxide. Here, we report the preparation of a copper-electrode onto which the po...
Autores principales: | , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2020
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7596083/ https://www.ncbi.nlm.nih.gov/pubmed/33122645 http://dx.doi.org/10.1038/s41467-020-19236-4 |
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author | Kang, Xinchen Li, Lili Sheveleva, Alena Han, Xue Li, Jiangnan Liu, Lifei Tuna, Floriana McInnes, Eric J. L. Han, Buxing Yang, Sihai Schröder, Martin |
author_facet | Kang, Xinchen Li, Lili Sheveleva, Alena Han, Xue Li, Jiangnan Liu, Lifei Tuna, Floriana McInnes, Eric J. L. Han, Buxing Yang, Sihai Schröder, Martin |
author_sort | Kang, Xinchen |
collection | PubMed |
description | Electrochemical reduction of carbon dioxide is a clean and highly attractive strategy for the production of organic products. However, this is hindered severely by the high negative potential required to activate carbon dioxide. Here, we report the preparation of a copper-electrode onto which the porous metal–organic framework [Cu(2)(L)] [H(4)L = 4,4′,4″,4′′′-(1,4-phenylenebis(pyridine-4,2,6-triyl))tetrabenzoic acid] can be deposited by electro-synthesis templated by an ionic liquid. This decorated electrode shows a remarkable onset potential for reduction of carbon dioxide to formic acid at −1.45 V vs. Ag/Ag(+), representing a low value for electro-reduction of carbon dioxide in an organic electrolyte. A current density of 65.8 mA·cm(−2) at −1.8 V vs. Ag/Ag(+) is observed with a Faradaic efficiency to formic acid of 90.5%. Electron paramagnetic resonance spectroscopy confirms that the templated electro-synthesis affords structural defects in the metal–organic framework film comprising uncoupled Cu(II) centres homogenously distributed throughout. These active sites promote catalytic performance as confirmed by computational modelling. |
format | Online Article Text |
id | pubmed-7596083 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-75960832020-11-10 Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode Kang, Xinchen Li, Lili Sheveleva, Alena Han, Xue Li, Jiangnan Liu, Lifei Tuna, Floriana McInnes, Eric J. L. Han, Buxing Yang, Sihai Schröder, Martin Nat Commun Article Electrochemical reduction of carbon dioxide is a clean and highly attractive strategy for the production of organic products. However, this is hindered severely by the high negative potential required to activate carbon dioxide. Here, we report the preparation of a copper-electrode onto which the porous metal–organic framework [Cu(2)(L)] [H(4)L = 4,4′,4″,4′′′-(1,4-phenylenebis(pyridine-4,2,6-triyl))tetrabenzoic acid] can be deposited by electro-synthesis templated by an ionic liquid. This decorated electrode shows a remarkable onset potential for reduction of carbon dioxide to formic acid at −1.45 V vs. Ag/Ag(+), representing a low value for electro-reduction of carbon dioxide in an organic electrolyte. A current density of 65.8 mA·cm(−2) at −1.8 V vs. Ag/Ag(+) is observed with a Faradaic efficiency to formic acid of 90.5%. Electron paramagnetic resonance spectroscopy confirms that the templated electro-synthesis affords structural defects in the metal–organic framework film comprising uncoupled Cu(II) centres homogenously distributed throughout. These active sites promote catalytic performance as confirmed by computational modelling. Nature Publishing Group UK 2020-10-29 /pmc/articles/PMC7596083/ /pubmed/33122645 http://dx.doi.org/10.1038/s41467-020-19236-4 Text en © The Author(s) 2020 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 Kang, Xinchen Li, Lili Sheveleva, Alena Han, Xue Li, Jiangnan Liu, Lifei Tuna, Floriana McInnes, Eric J. L. Han, Buxing Yang, Sihai Schröder, Martin Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode |
title | Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode |
title_full | Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode |
title_fullStr | Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode |
title_full_unstemmed | Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode |
title_short | Electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode |
title_sort | electro-reduction of carbon dioxide at low over-potential at a metal–organic framework decorated cathode |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7596083/ https://www.ncbi.nlm.nih.gov/pubmed/33122645 http://dx.doi.org/10.1038/s41467-020-19236-4 |
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