Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology

Autores
Muñoz, Fernando Francisco; Cabezas, Marcelo Daniel; Acuña, Leandro Marcelo; Leyva de Guglielmino, Ana Gabriela; Baker, Richard T.; Fuentes, Rodolfo Oscar
Año de publicación
2011
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In this work, nanostructured 1 wt % Pd/Gd2O3-CeO 2 (Pd/GDC) mixed oxide tubes with 90 mol % CeO2 were synthesized following a very simple, high yield procedure, and their properties were characterized by synchrotron radiation XRD, by X-ray absorption near-edge spectroscopy (XANES), and by scanning and high resolution electron microscopy (SEM and HRTEM). In situ XANES experiments were carried out under reducing conditions to investigate the reduction behavior of these novel tubular materials. The nanostructured mixed oxide tubes were found to have a cubic crystal phase (Fm3m space group) and large specific surface area (∼83 m 2 g-1). The tube walls were composed of nanoparticles with an average crystallite size of about 8 nm. The SEM and HRTEM results showed that individual tubes were composed of a curved sheet of these nanoparticles. Elemental analysis showed that Ce/Gd/Pd ratios appeared to be constant across space, suggesting compositional homogeneity in the samples. XANES results indicated that the extent of reduction of these materials was small. Nevertheless, the Ce3+ state was detected. These results suggest that Pd cations, most likely Pd2+, formed a Pd-Ce-Gd oxide solid solution and that the Pd2+ was stabilized against reduction in this phase. However, incorporation of the Pd (1 wt %) into the crystal lattice of the nanostructured tubes also appeared to destabilize Ce4+, favoring reduction to Ce3+ and giving rise to a significant increase in the reducibility of this material. Preliminary catalytic studies over Pd/GDC samples exhibited an improved catalytic activity toward CH4 oxidation compared to pure GDC (either nanotubes or nanopowders).
Fil: Muñoz, Fernando Francisco. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina
Fil: Cabezas, Marcelo Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina
Fil: Acuña, Leandro Marcelo. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Leyva de Guglielmino, Ana Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Baker, Richard T.. University of St. Andrews; Reino Unido
Fil: Fuentes, Rodolfo Oscar. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Materia
Nanotubes
Catalysis
GDC
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:11336/98346
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/98346
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphologyMuñoz, Fernando FranciscoCabezas, Marcelo DanielAcuña, Leandro MarceloLeyva de Guglielmino, Ana GabrielaBaker, Richard T.Fuentes, Rodolfo OscarNanotubesCatalysisGDChttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2In this work, nanostructured 1 wt % Pd/Gd2O3-CeO 2 (Pd/GDC) mixed oxide tubes with 90 mol % CeO2 were synthesized following a very simple, high yield procedure, and their properties were characterized by synchrotron radiation XRD, by X-ray absorption near-edge spectroscopy (XANES), and by scanning and high resolution electron microscopy (SEM and HRTEM). In situ XANES experiments were carried out under reducing conditions to investigate the reduction behavior of these novel tubular materials. The nanostructured mixed oxide tubes were found to have a cubic crystal phase (Fm3m space group) and large specific surface area (∼83 m 2 g-1). The tube walls were composed of nanoparticles with an average crystallite size of about 8 nm. The SEM and HRTEM results showed that individual tubes were composed of a curved sheet of these nanoparticles. Elemental analysis showed that Ce/Gd/Pd ratios appeared to be constant across space, suggesting compositional homogeneity in the samples. XANES results indicated that the extent of reduction of these materials was small. Nevertheless, the Ce3+ state was detected. These results suggest that Pd cations, most likely Pd2+, formed a Pd-Ce-Gd oxide solid solution and that the Pd2+ was stabilized against reduction in this phase. However, incorporation of the Pd (1 wt %) into the crystal lattice of the nanostructured tubes also appeared to destabilize Ce4+, favoring reduction to Ce3+ and giving rise to a significant increase in the reducibility of this material. Preliminary catalytic studies over Pd/GDC samples exhibited an improved catalytic activity toward CH4 oxidation compared to pure GDC (either nanotubes or nanopowders).Fil: Muñoz, Fernando Francisco. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; ArgentinaFil: Cabezas, Marcelo Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; ArgentinaFil: Acuña, Leandro Marcelo. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Leyva de Guglielmino, Ana Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; ArgentinaFil: Baker, Richard T.. University of St. Andrews; Reino UnidoFil: Fuentes, Rodolfo Oscar. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaAmerican Chemical Society2011-05info: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/11336/98346Muñoz, Fernando Francisco; Cabezas, Marcelo Daniel; Acuña, Leandro Marcelo; Leyva de Guglielmino, Ana Gabriela; Baker, Richard T.; et al.; Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology; American Chemical Society; Journal of Physical Chemistry C; 115; 17; 5-2011; 8744-87521932-7447CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/jp200667einfo:eu-repo/semantics/altIdentifier/doi/10.1021/jp200667einfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:55:55Zoai:ri.conicet.gov.ar:11336/98346instacron: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:34982025-10-22 11:55:55.497CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
title Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
spellingShingle Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
Muñoz, Fernando Francisco
Nanotubes
Catalysis
GDC
title_short Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
title_full Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
title_fullStr Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
title_full_unstemmed Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
title_sort Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology
dc.creator.none.fl_str_mv Muñoz, Fernando Francisco
Cabezas, Marcelo Daniel
Acuña, Leandro Marcelo
Leyva de Guglielmino, Ana Gabriela
Baker, Richard T.
Fuentes, Rodolfo Oscar
author Muñoz, Fernando Francisco
author_facet Muñoz, Fernando Francisco
Cabezas, Marcelo Daniel
Acuña, Leandro Marcelo
Leyva de Guglielmino, Ana Gabriela
Baker, Richard T.
Fuentes, Rodolfo Oscar
author_role author
author2 Cabezas, Marcelo Daniel
Acuña, Leandro Marcelo
Leyva de Guglielmino, Ana Gabriela
Baker, Richard T.
Fuentes, Rodolfo Oscar
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Nanotubes
Catalysis
GDC
topic Nanotubes
Catalysis
GDC
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 1 wt % Pd/Gd2O3-CeO 2 (Pd/GDC) mixed oxide tubes with 90 mol % CeO2 were synthesized following a very simple, high yield procedure, and their properties were characterized by synchrotron radiation XRD, by X-ray absorption near-edge spectroscopy (XANES), and by scanning and high resolution electron microscopy (SEM and HRTEM). In situ XANES experiments were carried out under reducing conditions to investigate the reduction behavior of these novel tubular materials. The nanostructured mixed oxide tubes were found to have a cubic crystal phase (Fm3m space group) and large specific surface area (∼83 m 2 g-1). The tube walls were composed of nanoparticles with an average crystallite size of about 8 nm. The SEM and HRTEM results showed that individual tubes were composed of a curved sheet of these nanoparticles. Elemental analysis showed that Ce/Gd/Pd ratios appeared to be constant across space, suggesting compositional homogeneity in the samples. XANES results indicated that the extent of reduction of these materials was small. Nevertheless, the Ce3+ state was detected. These results suggest that Pd cations, most likely Pd2+, formed a Pd-Ce-Gd oxide solid solution and that the Pd2+ was stabilized against reduction in this phase. However, incorporation of the Pd (1 wt %) into the crystal lattice of the nanostructured tubes also appeared to destabilize Ce4+, favoring reduction to Ce3+ and giving rise to a significant increase in the reducibility of this material. Preliminary catalytic studies over Pd/GDC samples exhibited an improved catalytic activity toward CH4 oxidation compared to pure GDC (either nanotubes or nanopowders).
Fil: Muñoz, Fernando Francisco. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina
Fil: Cabezas, Marcelo Daniel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina
Fil: Acuña, Leandro Marcelo. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Leyva de Guglielmino, Ana Gabriela. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Baker, Richard T.. University of St. Andrews; Reino Unido
Fil: Fuentes, Rodolfo Oscar. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
description In this work, nanostructured 1 wt % Pd/Gd2O3-CeO 2 (Pd/GDC) mixed oxide tubes with 90 mol % CeO2 were synthesized following a very simple, high yield procedure, and their properties were characterized by synchrotron radiation XRD, by X-ray absorption near-edge spectroscopy (XANES), and by scanning and high resolution electron microscopy (SEM and HRTEM). In situ XANES experiments were carried out under reducing conditions to investigate the reduction behavior of these novel tubular materials. The nanostructured mixed oxide tubes were found to have a cubic crystal phase (Fm3m space group) and large specific surface area (∼83 m 2 g-1). The tube walls were composed of nanoparticles with an average crystallite size of about 8 nm. The SEM and HRTEM results showed that individual tubes were composed of a curved sheet of these nanoparticles. Elemental analysis showed that Ce/Gd/Pd ratios appeared to be constant across space, suggesting compositional homogeneity in the samples. XANES results indicated that the extent of reduction of these materials was small. Nevertheless, the Ce3+ state was detected. These results suggest that Pd cations, most likely Pd2+, formed a Pd-Ce-Gd oxide solid solution and that the Pd2+ was stabilized against reduction in this phase. However, incorporation of the Pd (1 wt %) into the crystal lattice of the nanostructured tubes also appeared to destabilize Ce4+, favoring reduction to Ce3+ and giving rise to a significant increase in the reducibility of this material. Preliminary catalytic studies over Pd/GDC samples exhibited an improved catalytic activity toward CH4 oxidation compared to pure GDC (either nanotubes or nanopowders).
publishDate 2011
dc.date.none.fl_str_mv 2011-05
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/11336/98346
Muñoz, Fernando Francisco; Cabezas, Marcelo Daniel; Acuña, Leandro Marcelo; Leyva de Guglielmino, Ana Gabriela; Baker, Richard T.; et al.; Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology; American Chemical Society; Journal of Physical Chemistry C; 115; 17; 5-2011; 8744-8752
1932-7447
CONICET Digital
CONICET
url http://hdl.handle.net/11336/98346
identifier_str_mv Muñoz, Fernando Francisco; Cabezas, Marcelo Daniel; Acuña, Leandro Marcelo; Leyva de Guglielmino, Ana Gabriela; Baker, Richard T.; et al.; Structural properties and reduction behavior of novel nanostructured pd/gadolinia-doped ceria catalysts with tubular morphology; American Chemical Society; Journal of Physical Chemistry C; 115; 17; 5-2011; 8744-8752
1932-7447
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/jp200667e
info:eu-repo/semantics/altIdentifier/doi/10.1021/jp200667e
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
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 12.982451

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