Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO

Understanding how reaction conditions affect metal-support interactions in catalytic materials is one of the most challenging tasks in heterogeneous catalysis research. Metal nanoparticles and their supports often undergo changes in structure and oxidation state when exposed to reactants, hindering...

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Autores: Bezkrovnyi, O., Bruix Fusté, Albert, Blaumeiser, D., Piliai, L., Schötz, S., Bauer, T., Khalakhan, I., Skála, T., Matvija, P., Kraszkiewicz, P., Pawlyta, M., Vorokhta, M., Matolínová, I., Libuda, J., Neyman, Konstantin M., Kępiński, L.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2022
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/195927
Acceso en línea:https://hdl.handle.net/2445/195927
Access Level:acceso abierto
Palabra clave:Catalitzadors
Or
Òxids
Catalysts
Gold
Oxides
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spelling Metal-support interaction and charge distribution in ceria-supported Au particles exposed to COBezkrovnyi, O.Bruix Fusté, AlbertBlaumeiser, D.Piliai, L.Schötz, S.Bauer, T.Khalakhan, I.Skála, T.Matvija, P.Kraszkiewicz, P.Pawlyta, M.Vorokhta, M.Matolínová, I.Libuda, J.Neyman, Konstantin M.Kępiński, L.CatalitzadorsOrÒxidsCatalystsGoldOxidesUnderstanding how reaction conditions affect metal-support interactions in catalytic materials is one of the most challenging tasks in heterogeneous catalysis research. Metal nanoparticles and their supports often undergo changes in structure and oxidation state when exposed to reactants, hindering a straightforward understanding of the structure-activity relations using only ex situ or ultrahigh vacuum techniques. Overcoming these limitations, we explored the metal-support interaction between gold nanoparticles and ceria supports in ultrahigh vacuum and after exposure to CO. A combination of in situ methods (on powder and model Au/CeO2 samples) and theoretical calculations was applied to investigate the gold/ceria interface and its reactivity toward CO exposure. X-ray photoelectron spectroscopy measurements rationalized by first-principles calculations reveal a distinctly inhomogeneous charge distribution, with Au+ atoms in contact with the ceria substrate and neutral Au0 atoms at the surface of the Au nanoparticles. Exposure to CO partially reduces the ceria substrate, leading to electron transfer to the supported Au nanoparticles. Transferred electrons can delocalize among the neutral Au atoms of the particle or contribute to forming inert Auδ− atoms near oxygen vacancies at the ceria surface. This charge redistribution is consistent with the evolution of the vibrational frequencies of CO adsorbed on Au particles obtained using diffuse reflectance infrared Fourier transform spectroscopy.American Chemical Society2023202320222023info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion21 p.application/pdfhttps://hdl.handle.net/2445/195927Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésReproducció del document publicat a: https://doi.org/10.1021/acs.chemmater.2c01659Chemistry of Materials, 2022, vol. 34, num. 17, p. 7916-7936https://doi.org/10.1021/acs.chemmater.2c01659cc-by (c) Bezkrovnyi, O. et al., 2022http://creativecommons.org/licenses/by/3.0/es/info:eu-repo/semantics/openAccessoai:recercat.cat:2445/1959272026-05-29T05:05:01Z
dc.title.none.fl_str_mv Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
title Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
spellingShingle Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
Bezkrovnyi, O.
Catalitzadors
Or
Òxids
Catalysts
Gold
Oxides
title_short Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
title_full Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
title_fullStr Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
title_full_unstemmed Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
title_sort Metal-support interaction and charge distribution in ceria-supported Au particles exposed to CO
dc.creator.none.fl_str_mv Bezkrovnyi, O.
Bruix Fusté, Albert
Blaumeiser, D.
Piliai, L.
Schötz, S.
Bauer, T.
Khalakhan, I.
Skála, T.
Matvija, P.
Kraszkiewicz, P.
Pawlyta, M.
Vorokhta, M.
Matolínová, I.
Libuda, J.
Neyman, Konstantin M.
Kępiński, L.
author Bezkrovnyi, O.
author_facet Bezkrovnyi, O.
Bruix Fusté, Albert
Blaumeiser, D.
Piliai, L.
Schötz, S.
Bauer, T.
Khalakhan, I.
Skála, T.
Matvija, P.
Kraszkiewicz, P.
Pawlyta, M.
Vorokhta, M.
Matolínová, I.
Libuda, J.
Neyman, Konstantin M.
Kępiński, L.
author_role author
author2 Bruix Fusté, Albert
Blaumeiser, D.
Piliai, L.
Schötz, S.
Bauer, T.
Khalakhan, I.
Skála, T.
Matvija, P.
Kraszkiewicz, P.
Pawlyta, M.
Vorokhta, M.
Matolínová, I.
Libuda, J.
Neyman, Konstantin M.
Kępiński, L.
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Catalitzadors
Or
Òxids
Catalysts
Gold
Oxides
topic Catalitzadors
Or
Òxids
Catalysts
Gold
Oxides
description Understanding how reaction conditions affect metal-support interactions in catalytic materials is one of the most challenging tasks in heterogeneous catalysis research. Metal nanoparticles and their supports often undergo changes in structure and oxidation state when exposed to reactants, hindering a straightforward understanding of the structure-activity relations using only ex situ or ultrahigh vacuum techniques. Overcoming these limitations, we explored the metal-support interaction between gold nanoparticles and ceria supports in ultrahigh vacuum and after exposure to CO. A combination of in situ methods (on powder and model Au/CeO2 samples) and theoretical calculations was applied to investigate the gold/ceria interface and its reactivity toward CO exposure. X-ray photoelectron spectroscopy measurements rationalized by first-principles calculations reveal a distinctly inhomogeneous charge distribution, with Au+ atoms in contact with the ceria substrate and neutral Au0 atoms at the surface of the Au nanoparticles. Exposure to CO partially reduces the ceria substrate, leading to electron transfer to the supported Au nanoparticles. Transferred electrons can delocalize among the neutral Au atoms of the particle or contribute to forming inert Auδ− atoms near oxygen vacancies at the ceria surface. This charge redistribution is consistent with the evolution of the vibrational frequencies of CO adsorbed on Au particles obtained using diffuse reflectance infrared Fourier transform spectroscopy.
publishDate 2022
dc.date.none.fl_str_mv 2022
2023
2023
2023
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/195927
url https://hdl.handle.net/2445/195927
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.1021/acs.chemmater.2c01659
Chemistry of Materials, 2022, vol. 34, num. 17, p. 7916-7936
https://doi.org/10.1021/acs.chemmater.2c01659
dc.rights.none.fl_str_mv cc-by (c) Bezkrovnyi, O. et al., 2022
http://creativecommons.org/licenses/by/3.0/es/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by (c) Bezkrovnyi, O. et al., 2022
http://creativecommons.org/licenses/by/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 21 p.
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869416676767825920
score 15.81155

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