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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/82671
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CONICET Digital (CONICET) |
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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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1842268881427628032 |
score |
13.13397 |