Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation
Supported Pd/CeO2 catalytic systems have been widely investigated in the low-temperature oxidation of CO (LTO CO) due to the unique oxygen storage capacity and redox properties of the ceria support, which highly influence the structural, chemical and electronic state of Pd species. Herein, operando...
| Autores: | , , , , , , , , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2022 |
| País: | España |
| Institución: | Universitat Politècnica de Catalunya (UPC) |
| Repositorio: | UPCommons. Portal del coneixement obert de la UPC |
| Idioma: | inglés |
| OAI Identifier: | oai:upcommons.upc.edu:2117/386044 |
| Acceso en línea: | https://hdl.handle.net/2117/386044 https://dx.doi.org/10.3390/chemistry5010001 |
| Access Level: | acceso abierto |
| Palabra clave: | Catalysis Palladium catalyst Cerium oxide CO oxidation NAP-XPS Metal–support interaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
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Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidationGarcía de Andrés, Xènia|||0000-0003-0795-4168Soler Turu, Lluís|||0000-0003-1591-3366Vendrell Villafruela, Xavier|||0000-0003-4705-8253Serrano Carreño, M. Isabel|||0000-0002-4996-9280Herrera, FacundoPrat, JordiSolano Minuesa, EduardoTallarida, MassimoLlorca Piqué, Jordi|||0000-0002-7447-9582Escudero, CarlosCatalysisPalladium catalystCerium oxideCO oxidationNAP-XPSMetal–support interactionCatàlisiÀrees temàtiques de la UPC::Enginyeria químicaSupported Pd/CeO2 catalytic systems have been widely investigated in the low-temperature oxidation of CO (LTO CO) due to the unique oxygen storage capacity and redox properties of the ceria support, which highly influence the structural, chemical and electronic state of Pd species. Herein, operando near-ambient pressure XPS (NAP-XPS) technique has allowed the study of a conventional Pd/CeO2 catalyst surface during the CO oxidation reaction under experimental conditions closer to the actual catalytic reaction, unfeasible with other surface science techniques that demand UHV conditions. SEM, HRTEM and XRD analyses of the powder catalyst, prepared by conventional incipient wetness impregnation, reveal uniformly CeO2-loaded Pd NPs of less than 2 nm size, which generated an increase in oxygen vacancies with concomitant ceria reduction, as indicated by H2-TPR and Raman measurements. Adsorbed peroxide (O22-) species on the catalyst surface could also be detected by Raman spectra. Operando NAP-XPS results obtained at the ALBA Synchrotron Light Source revealed two kinds of Pd species under reaction conditions, namely PdOx and PdII ions in a PdxCe1-xO2-d solution, the latter one appearing to be crucial for the CO oxidation. By means of a non-destructive depth profile analysis using variable synchrotron excitation energies, the location and the role of these palladium species in the CO oxidation reaction could be clarified: PdOx was found to prevail on the upper surface layers of the metallic Pd supported NPs under CO, while under reaction mixture it was rapidly depleted from the surface, leaving a greater amount in the subsurface layers (7% vs. 12%, respectively). On the contrary, the PdxCe1-xO2-d phase, which was created at the Pd–CeO2 interface in contact with the gas environment, appeared to be predominant on the surface of the catalyst. Its presence was crucial for CO oxidation evolution, acting as a route through which active oxygen species could be transferred from ceria to Pd species for CO oxidation.Peer ReviewedMultidisciplinary Digital Publishing Institute (MDPI)20222022-12-2020232023-04-06journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/2117/386044https://dx.doi.org/10.3390/chemistry5010001reponame:UPCommons. Portal del coneixement obert de la UPCinstname:Universitat Politècnica de Catalunya (UPC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:upcommons.upc.edu:2117/3860442026-05-27T15:37:01Z |
| dc.title.none.fl_str_mv |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation |
| title |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation |
| spellingShingle |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation García de Andrés, Xènia|||0000-0003-0795-4168 Catalysis Palladium catalyst Cerium oxide CO oxidation NAP-XPS Metal–support interaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
| title_short |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation |
| title_full |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation |
| title_fullStr |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation |
| title_full_unstemmed |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation |
| title_sort |
Operando NAP-XPS studies of a ceria-supported Pd catalyst for CO oxidation |
| dc.creator.none.fl_str_mv |
García de Andrés, Xènia|||0000-0003-0795-4168 Soler Turu, Lluís|||0000-0003-1591-3366 Vendrell Villafruela, Xavier|||0000-0003-4705-8253 Serrano Carreño, M. Isabel|||0000-0002-4996-9280 Herrera, Facundo Prat, Jordi Solano Minuesa, Eduardo Tallarida, Massimo Llorca Piqué, Jordi|||0000-0002-7447-9582 Escudero, Carlos |
| author |
García de Andrés, Xènia|||0000-0003-0795-4168 |
| author_facet |
García de Andrés, Xènia|||0000-0003-0795-4168 Soler Turu, Lluís|||0000-0003-1591-3366 Vendrell Villafruela, Xavier|||0000-0003-4705-8253 Serrano Carreño, M. Isabel|||0000-0002-4996-9280 Herrera, Facundo Prat, Jordi Solano Minuesa, Eduardo Tallarida, Massimo Llorca Piqué, Jordi|||0000-0002-7447-9582 Escudero, Carlos |
| author_role |
author |
| author2 |
Soler Turu, Lluís|||0000-0003-1591-3366 Vendrell Villafruela, Xavier|||0000-0003-4705-8253 Serrano Carreño, M. Isabel|||0000-0002-4996-9280 Herrera, Facundo Prat, Jordi Solano Minuesa, Eduardo Tallarida, Massimo Llorca Piqué, Jordi|||0000-0002-7447-9582 Escudero, Carlos |
| author2_role |
author author author author author author author author author |
| dc.subject.none.fl_str_mv |
Catalysis Palladium catalyst Cerium oxide CO oxidation NAP-XPS Metal–support interaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
| topic |
Catalysis Palladium catalyst Cerium oxide CO oxidation NAP-XPS Metal–support interaction Catàlisi Àrees temàtiques de la UPC::Enginyeria química |
| description |
Supported Pd/CeO2 catalytic systems have been widely investigated in the low-temperature oxidation of CO (LTO CO) due to the unique oxygen storage capacity and redox properties of the ceria support, which highly influence the structural, chemical and electronic state of Pd species. Herein, operando near-ambient pressure XPS (NAP-XPS) technique has allowed the study of a conventional Pd/CeO2 catalyst surface during the CO oxidation reaction under experimental conditions closer to the actual catalytic reaction, unfeasible with other surface science techniques that demand UHV conditions. SEM, HRTEM and XRD analyses of the powder catalyst, prepared by conventional incipient wetness impregnation, reveal uniformly CeO2-loaded Pd NPs of less than 2 nm size, which generated an increase in oxygen vacancies with concomitant ceria reduction, as indicated by H2-TPR and Raman measurements. Adsorbed peroxide (O22-) species on the catalyst surface could also be detected by Raman spectra. Operando NAP-XPS results obtained at the ALBA Synchrotron Light Source revealed two kinds of Pd species under reaction conditions, namely PdOx and PdII ions in a PdxCe1-xO2-d solution, the latter one appearing to be crucial for the CO oxidation. By means of a non-destructive depth profile analysis using variable synchrotron excitation energies, the location and the role of these palladium species in the CO oxidation reaction could be clarified: PdOx was found to prevail on the upper surface layers of the metallic Pd supported NPs under CO, while under reaction mixture it was rapidly depleted from the surface, leaving a greater amount in the subsurface layers (7% vs. 12%, respectively). On the contrary, the PdxCe1-xO2-d phase, which was created at the Pd–CeO2 interface in contact with the gas environment, appeared to be predominant on the surface of the catalyst. Its presence was crucial for CO oxidation evolution, acting as a route through which active oxygen species could be transferred from ceria to Pd species for CO oxidation. |
| publishDate |
2022 |
| dc.date.none.fl_str_mv |
2022 2022-12-20 2023 2023-04-06 |
| dc.type.none.fl_str_mv |
journal article http://purl.org/coar/resource_type/c_6501 VoR http://purl.org/coar/version/c_970fb48d4fbd8a85 |
| dc.type.openaire.fl_str_mv |
info:eu-repo/semantics/article |
| format |
article |
| dc.identifier.none.fl_str_mv |
https://hdl.handle.net/2117/386044 https://dx.doi.org/10.3390/chemistry5010001 |
| url |
https://hdl.handle.net/2117/386044 https://dx.doi.org/10.3390/chemistry5010001 |
| dc.language.none.fl_str_mv |
Inglés eng |
| language_invalid_str_mv |
Inglés |
| language |
eng |
| dc.rights.none.fl_str_mv |
open access http://purl.org/coar/access_right/c_abf2 Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ |
| dc.rights.openaire.fl_str_mv |
info:eu-repo/semantics/openAccess |
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open access http://purl.org/coar/access_right/c_abf2 Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/ |
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openAccess |
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application/pdf |
| dc.publisher.none.fl_str_mv |
Multidisciplinary Digital Publishing Institute (MDPI) |
| publisher.none.fl_str_mv |
Multidisciplinary Digital Publishing Institute (MDPI) |
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reponame:UPCommons. Portal del coneixement obert de la UPC instname:Universitat Politècnica de Catalunya (UPC) |
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Universitat Politècnica de Catalunya (UPC) |
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UPCommons. Portal del coneixement obert de la UPC |
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UPCommons. Portal del coneixement obert de la UPC |
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