Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions

Autores
Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Albornoz, Cecilia Andrea; Leyva, A. G.; Sousa, N.; Figueiredo, F. M.
Año de publicación
2016
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
This work reports the synthesis of nanostructured Ce1-xNixO2-δ (x = 0.05, 0.1, 0.15 and 0.2) oxides prepared by cation complexation route and with the main objective of studying their redox properties using a combination of electron microscopy, synchrotron radiation X-ray diffraction (SR-XRD) and X-ray absorption near-edge spectroscopy (XANES). The Ce1-xNixO2-δ series of nanopowders maintain the cubic crystal structure (Fm3m space group) of pure ceria, with an average crystallite size of 5-7 nm indicated by XRD patterns and confirmed by transmission electron microscopy. In situ SR-XRD and XANES carried out under reducing (5% H2/He; 5% CO/He) and oxidizing (21%O2/N2) atmospheres at temperatures up to 500 °C show a Ni solubility limit close to 15 at.% in air at room temperature, decreasing to about 10 at.% after exposure to 5% H2/He atmosphere at 500 °C. At room temperature in air, the effect of Ni on the lattice parameter of Ce1-xNixO2-δ is negligible, whereas a marked expansion of the lattice is observed at 500 °C in reducing conditions. This is shown by XANES to be correlated with the reduction of up to 25% of Ce4+ cations to the much larger Ce3+, possibly accompanied by the formation of oxygen vacancies. The redox ability of the Ce4+/Ce3+ couple in nanocrystalline Ni-doped ceria is greatly enhanced in comparison to pure ceria or achieved by using other dopants (e.g. Gd, Tb or Pr), where it is limited to less than 5% of Ce cations.
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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Albornoz, Cecilia Andrea. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Leyva, A. G.. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Sousa, N.. University of Aveiro; Portugal
Fil: Figueiredo, F. M.. University of Aveiro; Portugal
Materia
NICKEL-SUBSTITUTED CERIA
NANOSTRUCTURED
XANES
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:11336/44244
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/44244
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditionsFuentes, Rodolfo OscarAcuña, Leandro MarceloAlbornoz, Cecilia AndreaLeyva, A. G.Sousa, N.Figueiredo, F. M.NICKEL-SUBSTITUTED CERIANANOSTRUCTUREDXANEShttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2This work reports the synthesis of nanostructured Ce1-xNixO2-δ (x = 0.05, 0.1, 0.15 and 0.2) oxides prepared by cation complexation route and with the main objective of studying their redox properties using a combination of electron microscopy, synchrotron radiation X-ray diffraction (SR-XRD) and X-ray absorption near-edge spectroscopy (XANES). The Ce1-xNixO2-δ series of nanopowders maintain the cubic crystal structure (Fm3m space group) of pure ceria, with an average crystallite size of 5-7 nm indicated by XRD patterns and confirmed by transmission electron microscopy. In situ SR-XRD and XANES carried out under reducing (5% H2/He; 5% CO/He) and oxidizing (21%O2/N2) atmospheres at temperatures up to 500 °C show a Ni solubility limit close to 15 at.% in air at room temperature, decreasing to about 10 at.% after exposure to 5% H2/He atmosphere at 500 °C. At room temperature in air, the effect of Ni on the lattice parameter of Ce1-xNixO2-δ is negligible, whereas a marked expansion of the lattice is observed at 500 °C in reducing conditions. This is shown by XANES to be correlated with the reduction of up to 25% of Ce4+ cations to the much larger Ce3+, possibly accompanied by the formation of oxygen vacancies. The redox ability of the Ce4+/Ce3+ couple in nanocrystalline Ni-doped ceria is greatly enhanced in comparison to pure ceria or achieved by using other dopants (e.g. Gd, Tb or Pr), where it is limited to less than 5% of Ce cations.Fil: Fuentes, Rodolfo Oscar. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; 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: Albornoz, Cecilia Andrea. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; ArgentinaFil: Leyva, A. G.. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; ArgentinaFil: Sousa, N.. University of Aveiro; PortugalFil: Figueiredo, F. M.. University of Aveiro; PortugalRoyal Society of Chemistry2016-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/44244Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Albornoz, Cecilia Andrea; Leyva, A. G.; Sousa, N.; et al.; Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions; Royal Society of Chemistry; RSC Advances; 6; 69; 7-2016; 64861-648702046-2069CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1039/C6RA14853Kinfo:eu-repo/semantics/altIdentifier/url/http://pubs.rsc.org/en/Content/ArticleLanding/2016/RA/C6RA14853Kinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T10:03:05Zoai:ri.conicet.gov.ar:11336/44244instacron: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 10:03:06.406CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
title Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
spellingShingle Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
Fuentes, Rodolfo Oscar
NICKEL-SUBSTITUTED CERIA
NANOSTRUCTURED
XANES
title_short Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
title_full Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
title_fullStr Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
title_full_unstemmed Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
title_sort Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions
dc.creator.none.fl_str_mv Fuentes, Rodolfo Oscar
Acuña, Leandro Marcelo
Albornoz, Cecilia Andrea
Leyva, A. G.
Sousa, N.
Figueiredo, F. M.
author Fuentes, Rodolfo Oscar
author_facet Fuentes, Rodolfo Oscar
Acuña, Leandro Marcelo
Albornoz, Cecilia Andrea
Leyva, A. G.
Sousa, N.
Figueiredo, F. M.
author_role author
author2 Acuña, Leandro Marcelo
Albornoz, Cecilia Andrea
Leyva, A. G.
Sousa, N.
Figueiredo, F. M.
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv NICKEL-SUBSTITUTED CERIA
NANOSTRUCTURED
XANES
topic NICKEL-SUBSTITUTED CERIA
NANOSTRUCTURED
XANES
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv This work reports the synthesis of nanostructured Ce1-xNixO2-δ (x = 0.05, 0.1, 0.15 and 0.2) oxides prepared by cation complexation route and with the main objective of studying their redox properties using a combination of electron microscopy, synchrotron radiation X-ray diffraction (SR-XRD) and X-ray absorption near-edge spectroscopy (XANES). The Ce1-xNixO2-δ series of nanopowders maintain the cubic crystal structure (Fm3m space group) of pure ceria, with an average crystallite size of 5-7 nm indicated by XRD patterns and confirmed by transmission electron microscopy. In situ SR-XRD and XANES carried out under reducing (5% H2/He; 5% CO/He) and oxidizing (21%O2/N2) atmospheres at temperatures up to 500 °C show a Ni solubility limit close to 15 at.% in air at room temperature, decreasing to about 10 at.% after exposure to 5% H2/He atmosphere at 500 °C. At room temperature in air, the effect of Ni on the lattice parameter of Ce1-xNixO2-δ is negligible, whereas a marked expansion of the lattice is observed at 500 °C in reducing conditions. This is shown by XANES to be correlated with the reduction of up to 25% of Ce4+ cations to the much larger Ce3+, possibly accompanied by the formation of oxygen vacancies. The redox ability of the Ce4+/Ce3+ couple in nanocrystalline Ni-doped ceria is greatly enhanced in comparison to pure ceria or achieved by using other dopants (e.g. Gd, Tb or Pr), where it is limited to less than 5% of Ce cations.
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. Ministerio de Defensa. Instituto de Investigaciones Científicas y Técnicas para la Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Albornoz, Cecilia Andrea. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Leyva, A. G.. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Nacional de San Martín. Escuela de Ciencia y Tecnología; Argentina
Fil: Sousa, N.. University of Aveiro; Portugal
Fil: Figueiredo, F. M.. University of Aveiro; Portugal
description This work reports the synthesis of nanostructured Ce1-xNixO2-δ (x = 0.05, 0.1, 0.15 and 0.2) oxides prepared by cation complexation route and with the main objective of studying their redox properties using a combination of electron microscopy, synchrotron radiation X-ray diffraction (SR-XRD) and X-ray absorption near-edge spectroscopy (XANES). The Ce1-xNixO2-δ series of nanopowders maintain the cubic crystal structure (Fm3m space group) of pure ceria, with an average crystallite size of 5-7 nm indicated by XRD patterns and confirmed by transmission electron microscopy. In situ SR-XRD and XANES carried out under reducing (5% H2/He; 5% CO/He) and oxidizing (21%O2/N2) atmospheres at temperatures up to 500 °C show a Ni solubility limit close to 15 at.% in air at room temperature, decreasing to about 10 at.% after exposure to 5% H2/He atmosphere at 500 °C. At room temperature in air, the effect of Ni on the lattice parameter of Ce1-xNixO2-δ is negligible, whereas a marked expansion of the lattice is observed at 500 °C in reducing conditions. This is shown by XANES to be correlated with the reduction of up to 25% of Ce4+ cations to the much larger Ce3+, possibly accompanied by the formation of oxygen vacancies. The redox ability of the Ce4+/Ce3+ couple in nanocrystalline Ni-doped ceria is greatly enhanced in comparison to pure ceria or achieved by using other dopants (e.g. Gd, Tb or Pr), where it is limited to less than 5% of Ce cations.
publishDate 2016
dc.date.none.fl_str_mv 2016-07
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/11336/44244
Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Albornoz, Cecilia Andrea; Leyva, A. G.; Sousa, N.; et al.; Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions; Royal Society of Chemistry; RSC Advances; 6; 69; 7-2016; 64861-64870
2046-2069
CONICET Digital
CONICET
url http://hdl.handle.net/11336/44244
identifier_str_mv Fuentes, Rodolfo Oscar; Acuña, Leandro Marcelo; Albornoz, Cecilia Andrea; Leyva, A. G.; Sousa, N.; et al.; Structural, physical and chemical properties of nanostructured nickel-substituted ceria oxides under reducing and oxidizing conditions; Royal Society of Chemistry; RSC Advances; 6; 69; 7-2016; 64861-64870
2046-2069
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/C6RA14853K
info:eu-repo/semantics/altIdentifier/url/http://pubs.rsc.org/en/Content/ArticleLanding/2016/RA/C6RA14853K
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
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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score 13.13397

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