Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties

Autores
Fortunato, Leandro Federico; Zubieta, Carolina Edith; Fuente, Silvia Andrea; Belelli, Patricia Gabriela; Ferullo, Ricardo
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We report a density functional theory (DFT) investigation on the interaction of tiny Aun (n = 1–5) clusters with the bare and hydroxylated (110) surfaces of goethite (α-FeOOH). Both adsorption and atom-by-atom nucleation processes were modeled. The adsorption is shown to be strong on the bare surface and takes place preferentially through the interaction of Au atoms with unsaturated surface oxygen anions, accompanied with an electronic charge transfer from the metal to the support. Au3, Au4 and Au5 planar structures resulted to be particularly stable due to polarization effects; indeed, Coulombic repulsion between basal Au atoms and surface oxygen anions promotes the displacement of the electronic density toward terminal Au atoms producing a Au+δ(basal)/Au−δ(terminal) polarization. On the hydroxylated surface, Au clusters adsorb more weakly with respect to the bare surface, mainly through monocoordinated surface hydroxyl groups and tricoordinated oxygen ions. Concerning the nucleation mechanism, while on the hydroxylated surface the nucleation energy is governed by the spin of the interacting systems, on the bare surface polarization effects seems to play a predominant role.
Fil: Fortunato, Leandro Federico. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
Fil: Zubieta, Carolina Edith. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
Fil: Fuente, Silvia Andrea. 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: Belelli, Patricia Gabriela. 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: Ferullo, Ricardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
Materia
ADSORPTION
DENSITY FUNCTIONAL CALCULATIONS
GOETHITE
POLARIZATION
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/55392
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/55392
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic propertiesFortunato, Leandro FedericoZubieta, Carolina EdithFuente, Silvia AndreaBelelli, Patricia GabrielaFerullo, RicardoADSORPTIONDENSITY FUNCTIONAL CALCULATIONSGOETHITEPOLARIZATIONhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1We report a density functional theory (DFT) investigation on the interaction of tiny Aun (n = 1–5) clusters with the bare and hydroxylated (110) surfaces of goethite (α-FeOOH). Both adsorption and atom-by-atom nucleation processes were modeled. The adsorption is shown to be strong on the bare surface and takes place preferentially through the interaction of Au atoms with unsaturated surface oxygen anions, accompanied with an electronic charge transfer from the metal to the support. Au3, Au4 and Au5 planar structures resulted to be particularly stable due to polarization effects; indeed, Coulombic repulsion between basal Au atoms and surface oxygen anions promotes the displacement of the electronic density toward terminal Au atoms producing a Au+δ(basal)/Au−δ(terminal) polarization. On the hydroxylated surface, Au clusters adsorb more weakly with respect to the bare surface, mainly through monocoordinated surface hydroxyl groups and tricoordinated oxygen ions. Concerning the nucleation mechanism, while on the hydroxylated surface the nucleation energy is governed by the spin of the interacting systems, on the bare surface polarization effects seems to play a predominant role.Fil: Fortunato, Leandro Federico. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; ArgentinaFil: Zubieta, Carolina Edith. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; ArgentinaFil: Fuente, Silvia Andrea. 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: Belelli, Patricia Gabriela. 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: Ferullo, Ricardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; ArgentinaElsevier Science2016-11-30info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/55392Fortunato, Leandro Federico; Zubieta, Carolina Edith; Fuente, Silvia Andrea; Belelli, Patricia Gabriela; Ferullo, Ricardo; Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties; Elsevier Science; Applied Surface Science; 387; 30-11-2016; 894-9010169-4332CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0169433216314386info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apsusc.2016.07.011info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:48:08Zoai:ri.conicet.gov.ar:11336/55392instacron: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 09:48:09.257CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
title Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
spellingShingle Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
Fortunato, Leandro Federico
ADSORPTION
DENSITY FUNCTIONAL CALCULATIONS
GOETHITE
POLARIZATION
title_short Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
title_full Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
title_fullStr Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
title_full_unstemmed Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
title_sort Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties
dc.creator.none.fl_str_mv Fortunato, Leandro Federico
Zubieta, Carolina Edith
Fuente, Silvia Andrea
Belelli, Patricia Gabriela
Ferullo, Ricardo
author Fortunato, Leandro Federico
author_facet Fortunato, Leandro Federico
Zubieta, Carolina Edith
Fuente, Silvia Andrea
Belelli, Patricia Gabriela
Ferullo, Ricardo
author_role author
author2 Zubieta, Carolina Edith
Fuente, Silvia Andrea
Belelli, Patricia Gabriela
Ferullo, Ricardo
author2_role author
author
author
author
dc.subject.none.fl_str_mv ADSORPTION
DENSITY FUNCTIONAL CALCULATIONS
GOETHITE
POLARIZATION
topic ADSORPTION
DENSITY FUNCTIONAL CALCULATIONS
GOETHITE
POLARIZATION
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv We report a density functional theory (DFT) investigation on the interaction of tiny Aun (n = 1–5) clusters with the bare and hydroxylated (110) surfaces of goethite (α-FeOOH). Both adsorption and atom-by-atom nucleation processes were modeled. The adsorption is shown to be strong on the bare surface and takes place preferentially through the interaction of Au atoms with unsaturated surface oxygen anions, accompanied with an electronic charge transfer from the metal to the support. Au3, Au4 and Au5 planar structures resulted to be particularly stable due to polarization effects; indeed, Coulombic repulsion between basal Au atoms and surface oxygen anions promotes the displacement of the electronic density toward terminal Au atoms producing a Au+δ(basal)/Au−δ(terminal) polarization. On the hydroxylated surface, Au clusters adsorb more weakly with respect to the bare surface, mainly through monocoordinated surface hydroxyl groups and tricoordinated oxygen ions. Concerning the nucleation mechanism, while on the hydroxylated surface the nucleation energy is governed by the spin of the interacting systems, on the bare surface polarization effects seems to play a predominant role.
Fil: Fortunato, Leandro Federico. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
Fil: Zubieta, Carolina Edith. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
Fil: Fuente, Silvia Andrea. 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: Belelli, Patricia Gabriela. 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: Ferullo, Ricardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Instituto de Química del Sur. Universidad Nacional del Sur. Departamento de Química. Instituto de Química del Sur; Argentina
description We report a density functional theory (DFT) investigation on the interaction of tiny Aun (n = 1–5) clusters with the bare and hydroxylated (110) surfaces of goethite (α-FeOOH). Both adsorption and atom-by-atom nucleation processes were modeled. The adsorption is shown to be strong on the bare surface and takes place preferentially through the interaction of Au atoms with unsaturated surface oxygen anions, accompanied with an electronic charge transfer from the metal to the support. Au3, Au4 and Au5 planar structures resulted to be particularly stable due to polarization effects; indeed, Coulombic repulsion between basal Au atoms and surface oxygen anions promotes the displacement of the electronic density toward terminal Au atoms producing a Au+δ(basal)/Au−δ(terminal) polarization. On the hydroxylated surface, Au clusters adsorb more weakly with respect to the bare surface, mainly through monocoordinated surface hydroxyl groups and tricoordinated oxygen ions. Concerning the nucleation mechanism, while on the hydroxylated surface the nucleation energy is governed by the spin of the interacting systems, on the bare surface polarization effects seems to play a predominant role.
publishDate 2016
dc.date.none.fl_str_mv 2016-11-30
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/11336/55392
Fortunato, Leandro Federico; Zubieta, Carolina Edith; Fuente, Silvia Andrea; Belelli, Patricia Gabriela; Ferullo, Ricardo; Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties; Elsevier Science; Applied Surface Science; 387; 30-11-2016; 894-901
0169-4332
CONICET Digital
CONICET
url http://hdl.handle.net/11336/55392
identifier_str_mv Fortunato, Leandro Federico; Zubieta, Carolina Edith; Fuente, Silvia Andrea; Belelli, Patricia Gabriela; Ferullo, Ricardo; Density functional studies of small Au clusters adsorbed on α-FeOOH: Structural and electronic properties; Elsevier Science; Applied Surface Science; 387; 30-11-2016; 894-901
0169-4332
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://www.sciencedirect.com/science/article/pii/S0169433216314386
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apsusc.2016.07.011
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv Elsevier Science
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
_version_ 1842268906627006464
score 13.13397

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