Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization

Autores
Poggio Fraccari, Eduardo Arístides; Irigoyen, Beatriz del Luján; Baronetti, Graciela Teresita; Mariño, Fernando Javier
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Experimental measurements by several techniques and density functional theory (DFT) calculations are combined to characterize Ce-Pr mixed oxides and deeply understand the influence of Pr dopant in their geometric and electronic structure, reducibility and catalytic behavior concerning the Water-gas Shift reaction (WGSR). Samples with nominal Pr dopant content of 0, 5, 15 and 50 at% (atomic percentage) are synthesized via urea decomposition method and subsequent calcination in air at 450 °C. X-ray diffraction characterization shows an increase of ceria lattice parameter for Pr loadings lower than 15 at%, which is consistent with a solid solution formation. X-ray photoelectron spectra indicate a surface enrichment in Pr cations and a diminution of Ce3+ surface concentration as Pr content increases. DFT calculations confirm the preferential reduction of Pr cations due to a single oxygen vacancy formation in Ce-Pr mixed oxides, and also a significant decrease in the energy needed for this O removal compare to that in pure CeO2. Both experimental measurements and DFT calculations evidence that the addition of Pr dopant to ceria promotes oxygen vacancies formation, redox properties and oxygen storage capacity (OSC). Even more, the same promoting effect of Pr in the WGSR intrinsic catalytic activity of Ce-Pr mixed oxides is observed.
Fil: Poggio Fraccari, Eduardo Arístides. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Irigoyen, Beatriz del Luján. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Baronetti, Graciela Teresita. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Mariño, Fernando Javier. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Materia
Ce-Pr Mixed Oxides
Dft Calculations
Oxygen Storage Capacity
Water Gas Shift Reaction
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/32189
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/32189
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterizationPoggio Fraccari, Eduardo ArístidesIrigoyen, Beatriz del LujánBaronetti, Graciela TeresitaMariño, Fernando JavierCe-Pr Mixed OxidesDft CalculationsOxygen Storage CapacityWater Gas Shift Reactionhttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2Experimental measurements by several techniques and density functional theory (DFT) calculations are combined to characterize Ce-Pr mixed oxides and deeply understand the influence of Pr dopant in their geometric and electronic structure, reducibility and catalytic behavior concerning the Water-gas Shift reaction (WGSR). Samples with nominal Pr dopant content of 0, 5, 15 and 50 at% (atomic percentage) are synthesized via urea decomposition method and subsequent calcination in air at 450 °C. X-ray diffraction characterization shows an increase of ceria lattice parameter for Pr loadings lower than 15 at%, which is consistent with a solid solution formation. X-ray photoelectron spectra indicate a surface enrichment in Pr cations and a diminution of Ce3+ surface concentration as Pr content increases. DFT calculations confirm the preferential reduction of Pr cations due to a single oxygen vacancy formation in Ce-Pr mixed oxides, and also a significant decrease in the energy needed for this O removal compare to that in pure CeO2. Both experimental measurements and DFT calculations evidence that the addition of Pr dopant to ceria promotes oxygen vacancies formation, redox properties and oxygen storage capacity (OSC). Even more, the same promoting effect of Pr in the WGSR intrinsic catalytic activity of Ce-Pr mixed oxides is observed.Fil: Poggio Fraccari, Eduardo Arístides. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; ArgentinaFil: Irigoyen, Beatriz del Luján. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; ArgentinaFil: Baronetti, Graciela Teresita. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; ArgentinaFil: Mariño, Fernando Javier. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; ArgentinaElsevier Science2014-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/32189Mariño, Fernando Javier; Baronetti, Graciela Teresita; Irigoyen, Beatriz del Luján; Poggio Fraccari, Eduardo Arístides; Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization; Elsevier Science; Applied Catalysis A: General; 485; 8-2014; 123-1320926-860XCONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2014.07.040info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0926860X14004700info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:07:59Zoai:ri.conicet.gov.ar:11336/32189instacron: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 10:07:59.465CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
title Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
spellingShingle Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
Poggio Fraccari, Eduardo Arístides
Ce-Pr Mixed Oxides
Dft Calculations
Oxygen Storage Capacity
Water Gas Shift Reaction
title_short Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
title_full Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
title_fullStr Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
title_full_unstemmed Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
title_sort Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization
dc.creator.none.fl_str_mv Poggio Fraccari, Eduardo Arístides
Irigoyen, Beatriz del Luján
Baronetti, Graciela Teresita
Mariño, Fernando Javier
author Poggio Fraccari, Eduardo Arístides
author_facet Poggio Fraccari, Eduardo Arístides
Irigoyen, Beatriz del Luján
Baronetti, Graciela Teresita
Mariño, Fernando Javier
author_role author
author2 Irigoyen, Beatriz del Luján
Baronetti, Graciela Teresita
Mariño, Fernando Javier
author2_role author
author
author
dc.subject.none.fl_str_mv Ce-Pr Mixed Oxides
Dft Calculations
Oxygen Storage Capacity
Water Gas Shift Reaction
topic Ce-Pr Mixed Oxides
Dft Calculations
Oxygen Storage Capacity
Water Gas Shift Reaction
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Experimental measurements by several techniques and density functional theory (DFT) calculations are combined to characterize Ce-Pr mixed oxides and deeply understand the influence of Pr dopant in their geometric and electronic structure, reducibility and catalytic behavior concerning the Water-gas Shift reaction (WGSR). Samples with nominal Pr dopant content of 0, 5, 15 and 50 at% (atomic percentage) are synthesized via urea decomposition method and subsequent calcination in air at 450 °C. X-ray diffraction characterization shows an increase of ceria lattice parameter for Pr loadings lower than 15 at%, which is consistent with a solid solution formation. X-ray photoelectron spectra indicate a surface enrichment in Pr cations and a diminution of Ce3+ surface concentration as Pr content increases. DFT calculations confirm the preferential reduction of Pr cations due to a single oxygen vacancy formation in Ce-Pr mixed oxides, and also a significant decrease in the energy needed for this O removal compare to that in pure CeO2. Both experimental measurements and DFT calculations evidence that the addition of Pr dopant to ceria promotes oxygen vacancies formation, redox properties and oxygen storage capacity (OSC). Even more, the same promoting effect of Pr in the WGSR intrinsic catalytic activity of Ce-Pr mixed oxides is observed.
Fil: Poggio Fraccari, Eduardo Arístides. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Irigoyen, Beatriz del Luján. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Baronetti, Graciela Teresita. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
Fil: Mariño, Fernando Javier. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles. Universidad de Buenos Aires. Facultad de Ingeniería. Instituto de Tecnologías del Hidrogeno y Energias Sostenibles; Argentina
description Experimental measurements by several techniques and density functional theory (DFT) calculations are combined to characterize Ce-Pr mixed oxides and deeply understand the influence of Pr dopant in their geometric and electronic structure, reducibility and catalytic behavior concerning the Water-gas Shift reaction (WGSR). Samples with nominal Pr dopant content of 0, 5, 15 and 50 at% (atomic percentage) are synthesized via urea decomposition method and subsequent calcination in air at 450 °C. X-ray diffraction characterization shows an increase of ceria lattice parameter for Pr loadings lower than 15 at%, which is consistent with a solid solution formation. X-ray photoelectron spectra indicate a surface enrichment in Pr cations and a diminution of Ce3+ surface concentration as Pr content increases. DFT calculations confirm the preferential reduction of Pr cations due to a single oxygen vacancy formation in Ce-Pr mixed oxides, and also a significant decrease in the energy needed for this O removal compare to that in pure CeO2. Both experimental measurements and DFT calculations evidence that the addition of Pr dopant to ceria promotes oxygen vacancies formation, redox properties and oxygen storage capacity (OSC). Even more, the same promoting effect of Pr in the WGSR intrinsic catalytic activity of Ce-Pr mixed oxides is observed.
publishDate 2014
dc.date.none.fl_str_mv 2014-08
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/11336/32189
Mariño, Fernando Javier; Baronetti, Graciela Teresita; Irigoyen, Beatriz del Luján; Poggio Fraccari, Eduardo Arístides; Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization; Elsevier Science; Applied Catalysis A: General; 485; 8-2014; 123-132
0926-860X
CONICET Digital
CONICET
url http://hdl.handle.net/11336/32189
identifier_str_mv Mariño, Fernando Javier; Baronetti, Graciela Teresita; Irigoyen, Beatriz del Luján; Poggio Fraccari, Eduardo Arístides; Ce-Pr mixed oxides as active supports for Water-gas Shift reaction: experimental and density functional theory characterization; Elsevier Science; Applied Catalysis A: General; 485; 8-2014; 123-132
0926-860X
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2014.07.040
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0926860X14004700
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
application/pdf
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
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