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Interfacial charge distributions in carbon-supported palladium catalysts

Controlling the charge transfer between a semiconducting catalyst carrier and the supported transition metal active phase represents an elite strategy for fine turning the electronic structure of the catalytic centers, hence their activity and selectivity. These phenomena have been theoretically and...

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Autores principales: Rao, Radhika G., Blume, Raoul, Hansen, Thomas W., Fuentes, Erika, Dreyer, Kathleen, Moldovan, Simona, Ersen, Ovidiu, Hibbitts, David D., Chabal, Yves J., Schlögl, Robert, Tessonnier, Jean-Philippe
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5569089/
https://www.ncbi.nlm.nih.gov/pubmed/28835704
http://dx.doi.org/10.1038/s41467-017-00421-x
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author Rao, Radhika G.
Blume, Raoul
Hansen, Thomas W.
Fuentes, Erika
Dreyer, Kathleen
Moldovan, Simona
Ersen, Ovidiu
Hibbitts, David D.
Chabal, Yves J.
Schlögl, Robert
Tessonnier, Jean-Philippe
author_facet Rao, Radhika G.
Blume, Raoul
Hansen, Thomas W.
Fuentes, Erika
Dreyer, Kathleen
Moldovan, Simona
Ersen, Ovidiu
Hibbitts, David D.
Chabal, Yves J.
Schlögl, Robert
Tessonnier, Jean-Philippe
author_sort Rao, Radhika G.
collection PubMed
description Controlling the charge transfer between a semiconducting catalyst carrier and the supported transition metal active phase represents an elite strategy for fine turning the electronic structure of the catalytic centers, hence their activity and selectivity. These phenomena have been theoretically and experimentally elucidated for oxide supports but remain poorly understood for carbons due to their complex nanoscale structure. Here, we combine advanced spectroscopy and microscopy on model Pd/C samples to decouple the electronic and surface chemistry effects on catalytic performance. Our investigations reveal trends between the charge distribution at the palladium–carbon interface and the metal’s selectivity for hydrogenation of multifunctional chemicals. These electronic effects are strong enough to affect the performance of large (~5 nm) Pd particles. Our results also demonstrate how simple thermal treatments can be used to tune the interfacial charge distribution, hereby providing a strategy to rationally design carbon-supported catalysts.
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spelling pubmed-55690892017-08-30 Interfacial charge distributions in carbon-supported palladium catalysts Rao, Radhika G. Blume, Raoul Hansen, Thomas W. Fuentes, Erika Dreyer, Kathleen Moldovan, Simona Ersen, Ovidiu Hibbitts, David D. Chabal, Yves J. Schlögl, Robert Tessonnier, Jean-Philippe Nat Commun Article Controlling the charge transfer between a semiconducting catalyst carrier and the supported transition metal active phase represents an elite strategy for fine turning the electronic structure of the catalytic centers, hence their activity and selectivity. These phenomena have been theoretically and experimentally elucidated for oxide supports but remain poorly understood for carbons due to their complex nanoscale structure. Here, we combine advanced spectroscopy and microscopy on model Pd/C samples to decouple the electronic and surface chemistry effects on catalytic performance. Our investigations reveal trends between the charge distribution at the palladium–carbon interface and the metal’s selectivity for hydrogenation of multifunctional chemicals. These electronic effects are strong enough to affect the performance of large (~5 nm) Pd particles. Our results also demonstrate how simple thermal treatments can be used to tune the interfacial charge distribution, hereby providing a strategy to rationally design carbon-supported catalysts. Nature Publishing Group UK 2017-08-24 /pmc/articles/PMC5569089/ /pubmed/28835704 http://dx.doi.org/10.1038/s41467-017-00421-x Text en © The Author(s) 2017 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
Rao, Radhika G.
Blume, Raoul
Hansen, Thomas W.
Fuentes, Erika
Dreyer, Kathleen
Moldovan, Simona
Ersen, Ovidiu
Hibbitts, David D.
Chabal, Yves J.
Schlögl, Robert
Tessonnier, Jean-Philippe
Interfacial charge distributions in carbon-supported palladium catalysts
title Interfacial charge distributions in carbon-supported palladium catalysts
title_full Interfacial charge distributions in carbon-supported palladium catalysts
title_fullStr Interfacial charge distributions in carbon-supported palladium catalysts
title_full_unstemmed Interfacial charge distributions in carbon-supported palladium catalysts
title_short Interfacial charge distributions in carbon-supported palladium catalysts
title_sort interfacial charge distributions in carbon-supported palladium catalysts
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5569089/
https://www.ncbi.nlm.nih.gov/pubmed/28835704
http://dx.doi.org/10.1038/s41467-017-00421-x
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