On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)

Autores
Branda, Maria Marta; Castellani, Norberto Jorge; Grau Crespo, Ricardo; de Leeuw, Nora H.; Hernandez, Norge C.; Sanz, Javier F.; Neyman, Konstantin M.; Illas, Francesc
Año de publicación
2009
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The electronic structure and oxidation state of atomic Au adsorbed on a perfect CeO2 (111) surface have been investigated in detail by means of periodic density functional theory-based calculations, using the LDA+U and GGA+U potentials for a broad range of U values, complemented with calculations employing the HSE06 hybrid functional. In addition, the effects of the lattice parameter a0 and of the starting point for the geometry optimization have also been analyzed. From the present results we suggest that the oxidation state of single Au atoms on CeO2 (111) predicted by LDA+U, GGA+U, and HSE06 density functional calculations is not conclusive and that the final picture strongly depends on the method chosen and on the construction of the surface model. In some cases we have been able to locate two well-defined states which are close in energy but with very different electronic structure and local geometries, one with Au fully oxidized and one with neutral Au. The energy difference between the two states is typically within the limits of the accuracy of the present exchange-correlation potentials, and therefore, a clear lowest-energy state cannot be identified. These results suggest the possibility of a dynamic distribution of Au0 and Au+ atomic species at the regular sites of the CeO2 (111) surface.
Fil: Branda, Maria Marta. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Castellani, Norberto Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Grau Crespo, Ricardo. University College London; Estados Unidos
Fil: de Leeuw, Nora H.. University College London; Estados Unidos
Fil: Hernandez, Norge C.. Universidad de Sevilla; España
Fil: Sanz, Javier F.. Universidad de Sevilla; España
Fil: Neyman, Konstantin M.. Institució Catalana de Recerca i Estudis Avancats; España. Universidad de Barcelona; España
Fil: Illas, Francesc. Universidad de Barcelona; España
Materia
Au
CeO2
DFT
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/69939
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/69939
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)Branda, Maria MartaCastellani, Norberto JorgeGrau Crespo, Ricardode Leeuw, Nora H.Hernandez, Norge C.Sanz, Javier F.Neyman, Konstantin M.Illas, FrancescAuCeO2DFThttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2The electronic structure and oxidation state of atomic Au adsorbed on a perfect CeO2 (111) surface have been investigated in detail by means of periodic density functional theory-based calculations, using the LDA+U and GGA+U potentials for a broad range of U values, complemented with calculations employing the HSE06 hybrid functional. In addition, the effects of the lattice parameter a0 and of the starting point for the geometry optimization have also been analyzed. From the present results we suggest that the oxidation state of single Au atoms on CeO2 (111) predicted by LDA+U, GGA+U, and HSE06 density functional calculations is not conclusive and that the final picture strongly depends on the method chosen and on the construction of the surface model. In some cases we have been able to locate two well-defined states which are close in energy but with very different electronic structure and local geometries, one with Au fully oxidized and one with neutral Au. The energy difference between the two states is typically within the limits of the accuracy of the present exchange-correlation potentials, and therefore, a clear lowest-energy state cannot be identified. These results suggest the possibility of a dynamic distribution of Au0 and Au+ atomic species at the regular sites of the CeO2 (111) surface.Fil: Branda, Maria Marta. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Castellani, Norberto Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; ArgentinaFil: Grau Crespo, Ricardo. University College London; Estados UnidosFil: de Leeuw, Nora H.. University College London; Estados UnidosFil: Hernandez, Norge C.. Universidad de Sevilla; EspañaFil: Sanz, Javier F.. Universidad de Sevilla; EspañaFil: Neyman, Konstantin M.. Institució Catalana de Recerca i Estudis Avancats; España. Universidad de Barcelona; EspañaFil: Illas, Francesc. Universidad de Barcelona; EspañaAmerican Institute of Physics2009-09-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/69939Branda, Maria Marta; Castellani, Norberto Jorge; Grau Crespo, Ricardo; de Leeuw, Nora H.; Hernandez, Norge C.; et al.; On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111); American Institute of Physics; Journal of Chemical Physics; 131; 9; 3-9-2009; 1-110021-96061089-7690CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/1.3216102info:eu-repo/semantics/altIdentifier/doi/10.1063/1.3216102info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:37:04Zoai:ri.conicet.gov.ar:11336/69939instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-29 09:37:04.566CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
title On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
spellingShingle On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
Branda, Maria Marta
Au
CeO2
DFT
title_short On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
title_full On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
title_fullStr On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
title_full_unstemmed On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
title_sort On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111)
dc.creator.none.fl_str_mv Branda, Maria Marta
Castellani, Norberto Jorge
Grau Crespo, Ricardo
de Leeuw, Nora H.
Hernandez, Norge C.
Sanz, Javier F.
Neyman, Konstantin M.
Illas, Francesc
author Branda, Maria Marta
author_facet Branda, Maria Marta
Castellani, Norberto Jorge
Grau Crespo, Ricardo
de Leeuw, Nora H.
Hernandez, Norge C.
Sanz, Javier F.
Neyman, Konstantin M.
Illas, Francesc
author_role author
author2 Castellani, Norberto Jorge
Grau Crespo, Ricardo
de Leeuw, Nora H.
Hernandez, Norge C.
Sanz, Javier F.
Neyman, Konstantin M.
Illas, Francesc
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Au
CeO2
DFT
topic Au
CeO2
DFT
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The electronic structure and oxidation state of atomic Au adsorbed on a perfect CeO2 (111) surface have been investigated in detail by means of periodic density functional theory-based calculations, using the LDA+U and GGA+U potentials for a broad range of U values, complemented with calculations employing the HSE06 hybrid functional. In addition, the effects of the lattice parameter a0 and of the starting point for the geometry optimization have also been analyzed. From the present results we suggest that the oxidation state of single Au atoms on CeO2 (111) predicted by LDA+U, GGA+U, and HSE06 density functional calculations is not conclusive and that the final picture strongly depends on the method chosen and on the construction of the surface model. In some cases we have been able to locate two well-defined states which are close in energy but with very different electronic structure and local geometries, one with Au fully oxidized and one with neutral Au. The energy difference between the two states is typically within the limits of the accuracy of the present exchange-correlation potentials, and therefore, a clear lowest-energy state cannot be identified. These results suggest the possibility of a dynamic distribution of Au0 and Au+ atomic species at the regular sites of the CeO2 (111) surface.
Fil: Branda, Maria Marta. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Castellani, Norberto Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Física del Sur. Universidad Nacional del Sur. Departamento de Física. Instituto de Física del Sur; Argentina
Fil: Grau Crespo, Ricardo. University College London; Estados Unidos
Fil: de Leeuw, Nora H.. University College London; Estados Unidos
Fil: Hernandez, Norge C.. Universidad de Sevilla; España
Fil: Sanz, Javier F.. Universidad de Sevilla; España
Fil: Neyman, Konstantin M.. Institució Catalana de Recerca i Estudis Avancats; España. Universidad de Barcelona; España
Fil: Illas, Francesc. Universidad de Barcelona; España
description The electronic structure and oxidation state of atomic Au adsorbed on a perfect CeO2 (111) surface have been investigated in detail by means of periodic density functional theory-based calculations, using the LDA+U and GGA+U potentials for a broad range of U values, complemented with calculations employing the HSE06 hybrid functional. In addition, the effects of the lattice parameter a0 and of the starting point for the geometry optimization have also been analyzed. From the present results we suggest that the oxidation state of single Au atoms on CeO2 (111) predicted by LDA+U, GGA+U, and HSE06 density functional calculations is not conclusive and that the final picture strongly depends on the method chosen and on the construction of the surface model. In some cases we have been able to locate two well-defined states which are close in energy but with very different electronic structure and local geometries, one with Au fully oxidized and one with neutral Au. The energy difference between the two states is typically within the limits of the accuracy of the present exchange-correlation potentials, and therefore, a clear lowest-energy state cannot be identified. These results suggest the possibility of a dynamic distribution of Au0 and Au+ atomic species at the regular sites of the CeO2 (111) surface.
publishDate 2009
dc.date.none.fl_str_mv 2009-09-03
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/69939
Branda, Maria Marta; Castellani, Norberto Jorge; Grau Crespo, Ricardo; de Leeuw, Nora H.; Hernandez, Norge C.; et al.; On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111); American Institute of Physics; Journal of Chemical Physics; 131; 9; 3-9-2009; 1-11
0021-9606
1089-7690
CONICET Digital
CONICET
url http://hdl.handle.net/11336/69939
identifier_str_mv Branda, Maria Marta; Castellani, Norberto Jorge; Grau Crespo, Ricardo; de Leeuw, Nora H.; Hernandez, Norge C.; et al.; On the difficulties of present theoretical models to predict the oxidation state of atomic Au adsorbed on regular sites of CeO2 (111); American Institute of Physics; Journal of Chemical Physics; 131; 9; 3-9-2009; 1-11
0021-9606
1089-7690
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/1.3216102
info:eu-repo/semantics/altIdentifier/doi/10.1063/1.3216102
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv American Institute of Physics
publisher.none.fl_str_mv American Institute of Physics
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.069144

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