Water dissociation at the Au/α-Fe2O3(0001) interface

Autores
Fuente, Silvia Andrea; Fortunato, Leandro Federico; Zubieta, Carolina Edith; Ferullo, Ricardo; Belelli, Patricia Gabriela
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The dissociative adsorption of water on a model catalyst formed by a Au5 cluster attached to the Fe-terminated (0001) surface of hematite (α-Fe2O3) was investigated within the density functional theory including an on-site Coulomb term (DFT + U). A flattened 2D-like structure was employed as supported gold particle. On clean hematite, the water molecule interacts with its O atom directly bound to a surface Fe ion. Conversely, in the most stable adsorption mode on Au5/hematite, it adsorbs in a multi-coordinated fashion at the metal-oxide interface and with one H atom oriented downward. Regarding the dissociative process, the isolated Au5 particle has a poor performance to activate one of the OH bonds (H2O → OH + H). However, when supported on hematite it becomes very active, having an activation barrier of only 0.09 eV. This process is even more favorable than on clean hematite. Thus, a very reactive site emerges at the metal-support interface. In this distinctive site, the water molecule is able to adsorb in a configuration (H-down) wherein one OH bond is strongly activated. An adsorbate-induced modification on the way that the flattened Au5 is anchored to the surface was observed, accompanied with changes in Au charges.
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: 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: 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
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
Materia
DFT
GOLD
HEMATITE
MODEL CATALYSTS
WGSR
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:11336/91359
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/91359
network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Water dissociation at the Au/α-Fe2O3(0001) interfaceFuente, Silvia AndreaFortunato, Leandro FedericoZubieta, Carolina EdithFerullo, RicardoBelelli, Patricia GabrielaDFTGOLDHEMATITEMODEL CATALYSTSWGSRhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The dissociative adsorption of water on a model catalyst formed by a Au5 cluster attached to the Fe-terminated (0001) surface of hematite (α-Fe2O3) was investigated within the density functional theory including an on-site Coulomb term (DFT + U). A flattened 2D-like structure was employed as supported gold particle. On clean hematite, the water molecule interacts with its O atom directly bound to a surface Fe ion. Conversely, in the most stable adsorption mode on Au5/hematite, it adsorbs in a multi-coordinated fashion at the metal-oxide interface and with one H atom oriented downward. Regarding the dissociative process, the isolated Au5 particle has a poor performance to activate one of the OH bonds (H2O → OH + H). However, when supported on hematite it becomes very active, having an activation barrier of only 0.09 eV. This process is even more favorable than on clean hematite. Thus, a very reactive site emerges at the metal-support interface. In this distinctive site, the water molecule is able to adsorb in a configuration (H-down) wherein one OH bond is strongly activated. An adsorbate-induced modification on the way that the flattened Au5 is anchored to the surface was observed, accompanied with changes in Au charges.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; ArgentinaFil: 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: 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; 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; ArgentinaElsevier B.V.2018-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/91359Fuente, Silvia Andrea; Fortunato, Leandro Federico; Zubieta, Carolina Edith; Ferullo, Ricardo; Belelli, Patricia Gabriela; Water dissociation at the Au/α-Fe2O3(0001) interface; Elsevier B.V.; Molecular Catalysis; 446; 2-2018; 10-222468-8231CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S2468823117306521info:eu-repo/semantics/altIdentifier/doi/10.1016/j.mcat.2017.12.011info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-29T11:43:57Zoai:ri.conicet.gov.ar:11336/91359instacron: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:34982025-10-29 11:43:57.778CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Water dissociation at the Au/α-Fe2O3(0001) interface
title Water dissociation at the Au/α-Fe2O3(0001) interface
spellingShingle Water dissociation at the Au/α-Fe2O3(0001) interface
Fuente, Silvia Andrea
DFT
GOLD
HEMATITE
MODEL CATALYSTS
WGSR
title_short Water dissociation at the Au/α-Fe2O3(0001) interface
title_full Water dissociation at the Au/α-Fe2O3(0001) interface
title_fullStr Water dissociation at the Au/α-Fe2O3(0001) interface
title_full_unstemmed Water dissociation at the Au/α-Fe2O3(0001) interface
title_sort Water dissociation at the Au/α-Fe2O3(0001) interface
dc.creator.none.fl_str_mv Fuente, Silvia Andrea
Fortunato, Leandro Federico
Zubieta, Carolina Edith
Ferullo, Ricardo
Belelli, Patricia Gabriela
author Fuente, Silvia Andrea
author_facet Fuente, Silvia Andrea
Fortunato, Leandro Federico
Zubieta, Carolina Edith
Ferullo, Ricardo
Belelli, Patricia Gabriela
author_role author
author2 Fortunato, Leandro Federico
Zubieta, Carolina Edith
Ferullo, Ricardo
Belelli, Patricia Gabriela
author2_role author
author
author
author
dc.subject.none.fl_str_mv DFT
GOLD
HEMATITE
MODEL CATALYSTS
WGSR
topic DFT
GOLD
HEMATITE
MODEL CATALYSTS
WGSR
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The dissociative adsorption of water on a model catalyst formed by a Au5 cluster attached to the Fe-terminated (0001) surface of hematite (α-Fe2O3) was investigated within the density functional theory including an on-site Coulomb term (DFT + U). A flattened 2D-like structure was employed as supported gold particle. On clean hematite, the water molecule interacts with its O atom directly bound to a surface Fe ion. Conversely, in the most stable adsorption mode on Au5/hematite, it adsorbs in a multi-coordinated fashion at the metal-oxide interface and with one H atom oriented downward. Regarding the dissociative process, the isolated Au5 particle has a poor performance to activate one of the OH bonds (H2O → OH + H). However, when supported on hematite it becomes very active, having an activation barrier of only 0.09 eV. This process is even more favorable than on clean hematite. Thus, a very reactive site emerges at the metal-support interface. In this distinctive site, the water molecule is able to adsorb in a configuration (H-down) wherein one OH bond is strongly activated. An adsorbate-induced modification on the way that the flattened Au5 is anchored to the surface was observed, accompanied with changes in Au charges.
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: 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: 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
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
description The dissociative adsorption of water on a model catalyst formed by a Au5 cluster attached to the Fe-terminated (0001) surface of hematite (α-Fe2O3) was investigated within the density functional theory including an on-site Coulomb term (DFT + U). A flattened 2D-like structure was employed as supported gold particle. On clean hematite, the water molecule interacts with its O atom directly bound to a surface Fe ion. Conversely, in the most stable adsorption mode on Au5/hematite, it adsorbs in a multi-coordinated fashion at the metal-oxide interface and with one H atom oriented downward. Regarding the dissociative process, the isolated Au5 particle has a poor performance to activate one of the OH bonds (H2O → OH + H). However, when supported on hematite it becomes very active, having an activation barrier of only 0.09 eV. This process is even more favorable than on clean hematite. Thus, a very reactive site emerges at the metal-support interface. In this distinctive site, the water molecule is able to adsorb in a configuration (H-down) wherein one OH bond is strongly activated. An adsorbate-induced modification on the way that the flattened Au5 is anchored to the surface was observed, accompanied with changes in Au charges.
publishDate 2018
dc.date.none.fl_str_mv 2018-02
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/11336/91359
Fuente, Silvia Andrea; Fortunato, Leandro Federico; Zubieta, Carolina Edith; Ferullo, Ricardo; Belelli, Patricia Gabriela; Water dissociation at the Au/α-Fe2O3(0001) interface; Elsevier B.V.; Molecular Catalysis; 446; 2-2018; 10-22
2468-8231
CONICET Digital
CONICET
url http://hdl.handle.net/11336/91359
identifier_str_mv Fuente, Silvia Andrea; Fortunato, Leandro Federico; Zubieta, Carolina Edith; Ferullo, Ricardo; Belelli, Patricia Gabriela; Water dissociation at the Au/α-Fe2O3(0001) interface; Elsevier B.V.; Molecular Catalysis; 446; 2-2018; 10-22
2468-8231
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/S2468823117306521
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.mcat.2017.12.011
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 B.V.
publisher.none.fl_str_mv Elsevier B.V.
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 13.10058

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