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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/69939
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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 Técnicas2025-09-03T09:46:05Zoai: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:34982025-09-03 09:46:05.692CONICET 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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1842268773411717120 |
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13.13397 |