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How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction

Development of reversible and stable catalysts for the electrochemical reduction of CO(2) is of great interest. Here, we elucidate the atomistic details of how a palladium electrocatalyst inhibits CO poisoning during both formic acid oxidation to carbon dioxide and carbon dioxide reduction to formic...

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Autores principales: Chen, Xiaoting, Granda-Marulanda, Laura P., McCrum, Ian T., Koper, Marc T. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8748733/
https://www.ncbi.nlm.nih.gov/pubmed/35013444
http://dx.doi.org/10.1038/s41467-021-27793-5
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author Chen, Xiaoting
Granda-Marulanda, Laura P.
McCrum, Ian T.
Koper, Marc T. M.
author_facet Chen, Xiaoting
Granda-Marulanda, Laura P.
McCrum, Ian T.
Koper, Marc T. M.
author_sort Chen, Xiaoting
collection PubMed
description Development of reversible and stable catalysts for the electrochemical reduction of CO(2) is of great interest. Here, we elucidate the atomistic details of how a palladium electrocatalyst inhibits CO poisoning during both formic acid oxidation to carbon dioxide and carbon dioxide reduction to formic acid. We compare results obtained with a platinum single-crystal electrode modified with and without a single monolayer of palladium. We combine (high-scan-rate) cyclic voltammetry with density functional theory to explain the absence of CO poisoning on the palladium-modified electrode. We show how the high formate coverage on the palladium-modified electrode protects the surface from poisoning during formic acid oxidation, and how the adsorption of CO precursor dictates the delayed poisoning during CO(2) reduction. The nature of the hydrogen adsorbed on the palladium-modified electrode is considerably different from platinum, supporting a model to explain the reversibility of this reaction. Our results help in designing catalysts for which CO poisoning needs to be avoided.
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spelling pubmed-87487332022-01-20 How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction Chen, Xiaoting Granda-Marulanda, Laura P. McCrum, Ian T. Koper, Marc T. M. Nat Commun Article Development of reversible and stable catalysts for the electrochemical reduction of CO(2) is of great interest. Here, we elucidate the atomistic details of how a palladium electrocatalyst inhibits CO poisoning during both formic acid oxidation to carbon dioxide and carbon dioxide reduction to formic acid. We compare results obtained with a platinum single-crystal electrode modified with and without a single monolayer of palladium. We combine (high-scan-rate) cyclic voltammetry with density functional theory to explain the absence of CO poisoning on the palladium-modified electrode. We show how the high formate coverage on the palladium-modified electrode protects the surface from poisoning during formic acid oxidation, and how the adsorption of CO precursor dictates the delayed poisoning during CO(2) reduction. The nature of the hydrogen adsorbed on the palladium-modified electrode is considerably different from platinum, supporting a model to explain the reversibility of this reaction. Our results help in designing catalysts for which CO poisoning needs to be avoided. Nature Publishing Group UK 2022-01-10 /pmc/articles/PMC8748733/ /pubmed/35013444 http://dx.doi.org/10.1038/s41467-021-27793-5 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
Chen, Xiaoting
Granda-Marulanda, Laura P.
McCrum, Ian T.
Koper, Marc T. M.
How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction
title How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction
title_full How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction
title_fullStr How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction
title_full_unstemmed How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction
title_short How palladium inhibits CO poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction
title_sort how palladium inhibits co poisoning during electrocatalytic formic acid oxidation and carbon dioxide reduction
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8748733/
https://www.ncbi.nlm.nih.gov/pubmed/35013444
http://dx.doi.org/10.1038/s41467-021-27793-5
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