Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties

Autores
Vecchietti, María Julia; Collins, Sebastián Enrique; Xu, Wenqian; Barrio, Laura; Stacchiola, Dario; Calatayud, Mónica; Tielens, Frederik; Delgado, Juan José; Bonivardi, Adrian Lionel
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The doping of CeO2 with different types of cations has been recognized as a significant factor in controlling the oxygen vacancies and improving the oxygen mobility. Thus, the catalytic properties of these materials might be determined by modifying the redox properties of ceria. A combined experimental and theoretical study of the redox properties of gallium-doped cerium dioxide is presented. Infrared spectroscopy and timeresolved X-ray diffraction were used for temperature programmed reduction (H2) and oxidation (with O2 and H2O) studies. Additionally, X-ray absorption near edge spectroscopy shows that only Ce4+ is reduced to Ce3+ in the ceria-gallia mixed oxides when annealed up to 623 K. The oxygen storage capacity (OSC) measurements show a pronounced enhancement on the reduction of ceria by gallium doping. Theoretical calculations by density functional theory (DFT) confirm the higher reducibility of gallium-doped ceria oxides and give a molecular description of the stabilization of the doped material. On the basis of infrared spectroscopic measurements, a novel mechanism is proposed for the surface reduction of Ce4+ to Ce3+ where Ga−H species are suggested to be directly involved in the process. In addition, the reoxidation by H2O was precluded in the galliumdoped ceria oxide.
Fil: Vecchietti, María Julia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico Para la Industria Química (i); Argentina
Fil: Collins, Sebastián Enrique. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico Para la Industria Química (i); Argentina
Fil: Xu, Wenqian. Brookhaven National Laboratory; Estados Unidos
Fil: Barrio, Laura. Brookhaven National Laboratory; Estados Unidos
Fil: Stacchiola, Dario. Brookhaven National Laboratory; Estados Unidos
Fil: Calatayud, Mónica. Universite Pierre Et Marie Curie; Francia
Fil: Tielens, Frederik. Universite Pierre Et Marie Curie; Francia
Fil: Delgado, Juan José. Universidad de Cadiz. Facultad de Ciencias. Departamento de Cs.de Los Materiales E Ing.metalurgica y Quim.inorg.; España
Fil: Bonivardi, Adrian Lionel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química (i); Argentina
Materia
Ga2o3
Infrared Spectroscopy
Xafs
Water Gas Shift Reaction
Dft
H2
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:11336/8756
Acceder
id CONICETDig_129882d7791b3e266b32fa27fdebd4ad
oai_identifier_str oai:ri.conicet.gov.ar:11336/8756
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox PropertiesVecchietti, María JuliaCollins, Sebastián EnriqueXu, WenqianBarrio, LauraStacchiola, DarioCalatayud, MónicaTielens, FrederikDelgado, Juan JoséBonivardi, Adrian LionelGa2o3Infrared SpectroscopyXafsWater Gas Shift ReactionDftH2https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The doping of CeO2 with different types of cations has been recognized as a significant factor in controlling the oxygen vacancies and improving the oxygen mobility. Thus, the catalytic properties of these materials might be determined by modifying the redox properties of ceria. A combined experimental and theoretical study of the redox properties of gallium-doped cerium dioxide is presented. Infrared spectroscopy and timeresolved X-ray diffraction were used for temperature programmed reduction (H2) and oxidation (with O2 and H2O) studies. Additionally, X-ray absorption near edge spectroscopy shows that only Ce4+ is reduced to Ce3+ in the ceria-gallia mixed oxides when annealed up to 623 K. The oxygen storage capacity (OSC) measurements show a pronounced enhancement on the reduction of ceria by gallium doping. Theoretical calculations by density functional theory (DFT) confirm the higher reducibility of gallium-doped ceria oxides and give a molecular description of the stabilization of the doped material. On the basis of infrared spectroscopic measurements, a novel mechanism is proposed for the surface reduction of Ce4+ to Ce3+ where Ga−H species are suggested to be directly involved in the process. In addition, the reoxidation by H2O was precluded in the galliumdoped ceria oxide.Fil: Vecchietti, María Julia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico Para la Industria Química (i); ArgentinaFil: Collins, Sebastián Enrique. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico Para la Industria Química (i); ArgentinaFil: Xu, Wenqian. Brookhaven National Laboratory; Estados UnidosFil: Barrio, Laura. Brookhaven National Laboratory; Estados UnidosFil: Stacchiola, Dario. Brookhaven National Laboratory; Estados UnidosFil: Calatayud, Mónica. Universite Pierre Et Marie Curie; FranciaFil: Tielens, Frederik. Universite Pierre Et Marie Curie; FranciaFil: Delgado, Juan José. Universidad de Cadiz. Facultad de Ciencias. Departamento de Cs.de Los Materiales E Ing.metalurgica y Quim.inorg.; EspañaFil: Bonivardi, Adrian Lionel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química (i); ArgentinaAmerican Chemical Society2013-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/8756Vecchietti, María Julia; Collins, Sebastián Enrique; Xu, Wenqian; Barrio, Laura; Stacchiola, Dario; et al.; Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties; American Chemical Society; Journal Of Physical Chemistry C; 117; 17; 4-2013; 8822-88311932-7447enginfo:eu-repo/semantics/altIdentifier/doi/10.1021/jp400285binfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/jp400285binfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:35:40Zoai:ri.conicet.gov.ar:11336/8756instacron: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 09:35:40.411CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
title Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
spellingShingle Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
Vecchietti, María Julia
Ga2o3
Infrared Spectroscopy
Xafs
Water Gas Shift Reaction
Dft
H2
title_short Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
title_full Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
title_fullStr Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
title_full_unstemmed Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
title_sort Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties
dc.creator.none.fl_str_mv Vecchietti, María Julia
Collins, Sebastián Enrique
Xu, Wenqian
Barrio, Laura
Stacchiola, Dario
Calatayud, Mónica
Tielens, Frederik
Delgado, Juan José
Bonivardi, Adrian Lionel
author Vecchietti, María Julia
author_facet Vecchietti, María Julia
Collins, Sebastián Enrique
Xu, Wenqian
Barrio, Laura
Stacchiola, Dario
Calatayud, Mónica
Tielens, Frederik
Delgado, Juan José
Bonivardi, Adrian Lionel
author_role author
author2 Collins, Sebastián Enrique
Xu, Wenqian
Barrio, Laura
Stacchiola, Dario
Calatayud, Mónica
Tielens, Frederik
Delgado, Juan José
Bonivardi, Adrian Lionel
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Ga2o3
Infrared Spectroscopy
Xafs
Water Gas Shift Reaction
Dft
H2
topic Ga2o3
Infrared Spectroscopy
Xafs
Water Gas Shift Reaction
Dft
H2
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 doping of CeO2 with different types of cations has been recognized as a significant factor in controlling the oxygen vacancies and improving the oxygen mobility. Thus, the catalytic properties of these materials might be determined by modifying the redox properties of ceria. A combined experimental and theoretical study of the redox properties of gallium-doped cerium dioxide is presented. Infrared spectroscopy and timeresolved X-ray diffraction were used for temperature programmed reduction (H2) and oxidation (with O2 and H2O) studies. Additionally, X-ray absorption near edge spectroscopy shows that only Ce4+ is reduced to Ce3+ in the ceria-gallia mixed oxides when annealed up to 623 K. The oxygen storage capacity (OSC) measurements show a pronounced enhancement on the reduction of ceria by gallium doping. Theoretical calculations by density functional theory (DFT) confirm the higher reducibility of gallium-doped ceria oxides and give a molecular description of the stabilization of the doped material. On the basis of infrared spectroscopic measurements, a novel mechanism is proposed for the surface reduction of Ce4+ to Ce3+ where Ga−H species are suggested to be directly involved in the process. In addition, the reoxidation by H2O was precluded in the galliumdoped ceria oxide.
Fil: Vecchietti, María Julia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico Para la Industria Química (i); Argentina
Fil: Collins, Sebastián Enrique. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico Para la Industria Química (i); Argentina
Fil: Xu, Wenqian. Brookhaven National Laboratory; Estados Unidos
Fil: Barrio, Laura. Brookhaven National Laboratory; Estados Unidos
Fil: Stacchiola, Dario. Brookhaven National Laboratory; Estados Unidos
Fil: Calatayud, Mónica. Universite Pierre Et Marie Curie; Francia
Fil: Tielens, Frederik. Universite Pierre Et Marie Curie; Francia
Fil: Delgado, Juan José. Universidad de Cadiz. Facultad de Ciencias. Departamento de Cs.de Los Materiales E Ing.metalurgica y Quim.inorg.; España
Fil: Bonivardi, Adrian Lionel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química (i); Argentina
description The doping of CeO2 with different types of cations has been recognized as a significant factor in controlling the oxygen vacancies and improving the oxygen mobility. Thus, the catalytic properties of these materials might be determined by modifying the redox properties of ceria. A combined experimental and theoretical study of the redox properties of gallium-doped cerium dioxide is presented. Infrared spectroscopy and timeresolved X-ray diffraction were used for temperature programmed reduction (H2) and oxidation (with O2 and H2O) studies. Additionally, X-ray absorption near edge spectroscopy shows that only Ce4+ is reduced to Ce3+ in the ceria-gallia mixed oxides when annealed up to 623 K. The oxygen storage capacity (OSC) measurements show a pronounced enhancement on the reduction of ceria by gallium doping. Theoretical calculations by density functional theory (DFT) confirm the higher reducibility of gallium-doped ceria oxides and give a molecular description of the stabilization of the doped material. On the basis of infrared spectroscopic measurements, a novel mechanism is proposed for the surface reduction of Ce4+ to Ce3+ where Ga−H species are suggested to be directly involved in the process. In addition, the reoxidation by H2O was precluded in the galliumdoped ceria oxide.
publishDate 2013
dc.date.none.fl_str_mv 2013-04
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/11336/8756
Vecchietti, María Julia; Collins, Sebastián Enrique; Xu, Wenqian; Barrio, Laura; Stacchiola, Dario; et al.; Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties; American Chemical Society; Journal Of Physical Chemistry C; 117; 17; 4-2013; 8822-8831
1932-7447
url http://hdl.handle.net/11336/8756
identifier_str_mv Vecchietti, María Julia; Collins, Sebastián Enrique; Xu, Wenqian; Barrio, Laura; Stacchiola, Dario; et al.; Surface Reduction Mechanism of Cerium-Gallium Mixed Oxides with Enhanced Redox Properties; American Chemical Society; Journal Of Physical Chemistry C; 117; 17; 4-2013; 8822-8831
1932-7447
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/jp400285b
info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/jp400285b
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
application/pdf
application/pdf
application/pdf
application/pdf
application/pdf
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 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 13.070432

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