Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion

Autores
Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Leyva, A. Gabriela; Baker, Richard T.; Pan, Huiyan; Chen, Xiaowei; Delgado Jaén, Juan J.
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In this work, nanostructured Ce0.9Gd0.1O2-δ (GDC) and Ce0.9Pr0.1O2-δ (PrDC) spheres previously obtained by microwave assisted hydrothermal homogeneous co-precipitation were impregnated with 1 wt% Pd by the incipient wetness impregnation by an aqueous Pd2+ solution. Their properties were characterized by synchrotron radiation X-ray diffraction (SR-XRD), X-ray absorption near-edge spectroscopy (XANES) and scanning and high resolution electron microscopy with X-ray spectroscopy. Spherical particles with average diameters around 200 nm were found to consist of crystallites of average size, 10 nm, with small particles of PdO finely dispersed over the sphere surface. In situ XRD and XANES experiments were carried out under reducing and oxidizing conditions in order to investigate the redox behaviour of these materials and to evaluate the effect of Pd loading on the oxidation state of Ce. All of the lanthanide-doped ceria (LnDC) supports were found to have a cubic crystal structure (Fm3m space group). An increase in lattice parameters was observed under reducing conditions which was attributed to the reduction of Ce4+ ions to the larger Ce3+ ions, and to the associated increase in oxygen vacancy (VO) concentration. Addition of Pd to the LnDC spheres increased their Ce3+ content. Finally, catalytic tests for CH4 combustion were performed on the LnDC and Pd/LnDC nanocatalysts. The best performance was observed in samples with 1 wt% Pd loading, which exhibited T50 values (temperature at which 50% of CH4 conversion was reached) close to 310 °C. These values are 220 °C and 260 °C lower than those obtained for nanostructured PrDC and GDC spheres alone, respectively.
Fil: Fuentes, Rodolfo Oscar. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Acuña, Leandro Marcelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentina
Fil: Leyva, A. Gabriela. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Baker, Richard T.. University of St. Andrews; Reino Unido
Fil: Pan, Huiyan. Universidad de Cádiz; España
Fil: Chen, Xiaowei. Universidad de Cádiz; España
Fil: Delgado Jaén, Juan J.. Universidad de Cádiz; España
Materia
NANOMATERIALS
CERIA
CATALYSTS
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:11336/82671

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network_name_str CONICET Digital (CONICET)
spelling Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustionFuentes, Rodolfo OscarAcuña, Leandro MarceloLeyva, A. GabrielaBaker, Richard T.Pan, HuiyanChen, XiaoweiDelgado Jaén, Juan J.NANOMATERIALSCERIACATALYSTShttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2In this work, nanostructured Ce0.9Gd0.1O2-δ (GDC) and Ce0.9Pr0.1O2-δ (PrDC) spheres previously obtained by microwave assisted hydrothermal homogeneous co-precipitation were impregnated with 1 wt% Pd by the incipient wetness impregnation by an aqueous Pd2+ solution. Their properties were characterized by synchrotron radiation X-ray diffraction (SR-XRD), X-ray absorption near-edge spectroscopy (XANES) and scanning and high resolution electron microscopy with X-ray spectroscopy. Spherical particles with average diameters around 200 nm were found to consist of crystallites of average size, 10 nm, with small particles of PdO finely dispersed over the sphere surface. In situ XRD and XANES experiments were carried out under reducing and oxidizing conditions in order to investigate the redox behaviour of these materials and to evaluate the effect of Pd loading on the oxidation state of Ce. All of the lanthanide-doped ceria (LnDC) supports were found to have a cubic crystal structure (Fm3m space group). An increase in lattice parameters was observed under reducing conditions which was attributed to the reduction of Ce4+ ions to the larger Ce3+ ions, and to the associated increase in oxygen vacancy (VO) concentration. Addition of Pd to the LnDC spheres increased their Ce3+ content. Finally, catalytic tests for CH4 combustion were performed on the LnDC and Pd/LnDC nanocatalysts. The best performance was observed in samples with 1 wt% Pd loading, which exhibited T50 values (temperature at which 50% of CH4 conversion was reached) close to 310 °C. These values are 220 °C and 260 °C lower than those obtained for nanostructured PrDC and GDC spheres alone, respectively.Fil: Fuentes, Rodolfo Oscar. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Acuña, Leandro Marcelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; ArgentinaFil: Leyva, A. Gabriela. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; ArgentinaFil: Baker, Richard T.. University of St. Andrews; Reino UnidoFil: Pan, Huiyan. Universidad de Cádiz; EspañaFil: Chen, Xiaowei. Universidad de Cádiz; EspañaFil: Delgado Jaén, Juan J.. Universidad de Cádiz; EspañaRoyal Society of Chemistry2018-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/82671Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Leyva, A. Gabriela; Baker, Richard T.; Pan, Huiyan; et al.; Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion; Royal Society of Chemistry; Journal of Materials Chemistry A; 6; 17; 3-2018; 7488-74992050-7488CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1039/c8ta00203ginfo:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2018/TA/C8TA00203Ginfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:47:47Zoai:ri.conicet.gov.ar:11336/82671instacron: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 09:47:47.394CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
title Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
spellingShingle Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
Fuentes, Rodolfo Oscar
NANOMATERIALS
CERIA
CATALYSTS
title_short Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
title_full Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
title_fullStr Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
title_full_unstemmed Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
title_sort Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion
dc.creator.none.fl_str_mv Fuentes, Rodolfo Oscar
Acuña, Leandro Marcelo
Leyva, A. Gabriela
Baker, Richard T.
Pan, Huiyan
Chen, Xiaowei
Delgado Jaén, Juan J.
author Fuentes, Rodolfo Oscar
author_facet Fuentes, Rodolfo Oscar
Acuña, Leandro Marcelo
Leyva, A. Gabriela
Baker, Richard T.
Pan, Huiyan
Chen, Xiaowei
Delgado Jaén, Juan J.
author_role author
author2 Acuña, Leandro Marcelo
Leyva, A. Gabriela
Baker, Richard T.
Pan, Huiyan
Chen, Xiaowei
Delgado Jaén, Juan J.
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv NANOMATERIALS
CERIA
CATALYSTS
topic NANOMATERIALS
CERIA
CATALYSTS
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv In this work, nanostructured Ce0.9Gd0.1O2-δ (GDC) and Ce0.9Pr0.1O2-δ (PrDC) spheres previously obtained by microwave assisted hydrothermal homogeneous co-precipitation were impregnated with 1 wt% Pd by the incipient wetness impregnation by an aqueous Pd2+ solution. Their properties were characterized by synchrotron radiation X-ray diffraction (SR-XRD), X-ray absorption near-edge spectroscopy (XANES) and scanning and high resolution electron microscopy with X-ray spectroscopy. Spherical particles with average diameters around 200 nm were found to consist of crystallites of average size, 10 nm, with small particles of PdO finely dispersed over the sphere surface. In situ XRD and XANES experiments were carried out under reducing and oxidizing conditions in order to investigate the redox behaviour of these materials and to evaluate the effect of Pd loading on the oxidation state of Ce. All of the lanthanide-doped ceria (LnDC) supports were found to have a cubic crystal structure (Fm3m space group). An increase in lattice parameters was observed under reducing conditions which was attributed to the reduction of Ce4+ ions to the larger Ce3+ ions, and to the associated increase in oxygen vacancy (VO) concentration. Addition of Pd to the LnDC spheres increased their Ce3+ content. Finally, catalytic tests for CH4 combustion were performed on the LnDC and Pd/LnDC nanocatalysts. The best performance was observed in samples with 1 wt% Pd loading, which exhibited T50 values (temperature at which 50% of CH4 conversion was reached) close to 310 °C. These values are 220 °C and 260 °C lower than those obtained for nanostructured PrDC and GDC spheres alone, respectively.
Fil: Fuentes, Rodolfo Oscar. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Acuña, Leandro Marcelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentina
Fil: Leyva, A. Gabriela. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Baker, Richard T.. University of St. Andrews; Reino Unido
Fil: Pan, Huiyan. Universidad de Cádiz; España
Fil: Chen, Xiaowei. Universidad de Cádiz; España
Fil: Delgado Jaén, Juan J.. Universidad de Cádiz; España
description In this work, nanostructured Ce0.9Gd0.1O2-δ (GDC) and Ce0.9Pr0.1O2-δ (PrDC) spheres previously obtained by microwave assisted hydrothermal homogeneous co-precipitation were impregnated with 1 wt% Pd by the incipient wetness impregnation by an aqueous Pd2+ solution. Their properties were characterized by synchrotron radiation X-ray diffraction (SR-XRD), X-ray absorption near-edge spectroscopy (XANES) and scanning and high resolution electron microscopy with X-ray spectroscopy. Spherical particles with average diameters around 200 nm were found to consist of crystallites of average size, 10 nm, with small particles of PdO finely dispersed over the sphere surface. In situ XRD and XANES experiments were carried out under reducing and oxidizing conditions in order to investigate the redox behaviour of these materials and to evaluate the effect of Pd loading on the oxidation state of Ce. All of the lanthanide-doped ceria (LnDC) supports were found to have a cubic crystal structure (Fm3m space group). An increase in lattice parameters was observed under reducing conditions which was attributed to the reduction of Ce4+ ions to the larger Ce3+ ions, and to the associated increase in oxygen vacancy (VO) concentration. Addition of Pd to the LnDC spheres increased their Ce3+ content. Finally, catalytic tests for CH4 combustion were performed on the LnDC and Pd/LnDC nanocatalysts. The best performance was observed in samples with 1 wt% Pd loading, which exhibited T50 values (temperature at which 50% of CH4 conversion was reached) close to 310 °C. These values are 220 °C and 260 °C lower than those obtained for nanostructured PrDC and GDC spheres alone, respectively.
publishDate 2018
dc.date.none.fl_str_mv 2018-03
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/11336/82671
Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Leyva, A. Gabriela; Baker, Richard T.; Pan, Huiyan; et al.; Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion; Royal Society of Chemistry; Journal of Materials Chemistry A; 6; 17; 3-2018; 7488-7499
2050-7488
CONICET Digital
CONICET
url http://hdl.handle.net/11336/82671
identifier_str_mv Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Leyva, A. Gabriela; Baker, Richard T.; Pan, Huiyan; et al.; Physicochemical properties of nanostructured Pd/lanthanide-doped ceria spheres with high catalytic activity for CH4 combustion; Royal Society of Chemistry; Journal of Materials Chemistry A; 6; 17; 3-2018; 7488-7499
2050-7488
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1039/c8ta00203g
info:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2018/TA/C8TA00203G
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
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
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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