Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ

Autores
Heras Juaristi, Gemma; Amador, Ulises; Romero de Paz, Julio; Fuentes, Rodolfo Oscar; Chinelatto, Adilson L.; Ritter, Clemens; Fagg, Duncan P.; Pérez Coll, Domingo; Mather, Glenn C.
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ -BaPrO 3-δ perovskite system, of interest for high-temperature electrochemical applications involving mixed protonic-electronic conductivity, forms a solid-solution with a wide interval of Ba substoichiometry in the range Ba(Ce 0.2 Zr 0.7 ) 1-x Pr x Y 0.1 O 3-δ , 0 ≤ x ≤ 1. Structural phase transitions mapped as a function of temperature and composition by high-resolution neutron powder diffraction and synchrotron X-ray diffraction reveal higher symmetry for lower Pr content and higher temperatures, with the largest stability field observed for rhombohedral symmetry (space group, R3c). Rietveld refinement, supported by magnetic-susceptibility measurements, indicates that partitioning of the B-site cations over the A and B perovskite sites compensates Ba substoichiometry in preference to A-site vacancy formation and that multiple cations are distributed over both sites. Electron-hole transport dominates electrical conductivity in both wet and dry oxidizing conditions, with total conductivity reaching a value of 0.5 S cm -1 for the x = 1 end-member in dry air at 1173 K. Higher electrical conductivity and the displacement of oxygen loss to higher temperatures with increasing Pr content both reflect the role of Pr in promoting hole formation at the expense of oxygen vacancies. In more reducing conditions (N 2 ) and at low Pr contents, conductivity is higher in humidified atmospheres (0.023 atm pH 2 O) indicating a protonic contribution to transport, whereas the greater electron-hole conductivity with increasing Pr content results in lower conductivity in humidified N 2 due to the creation of protonic defects and the consumption of holes.
Fil: Heras Juaristi, Gemma. Instituto de Ceramica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; España
Fil: Amador, Ulises. Universidad CEU-San Pablo; España
Fil: Romero de Paz, Julio. Universidad Complutense de Madrid; España
Fil: Fuentes, Rodolfo Oscar. Comisión Nacional de Energía Atómica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Chinelatto, Adilson L.. Universidade Estadual de Ponta Grossa; Brasil
Fil: Ritter, Clemens. Institut Laue-Langevin; Francia
Fil: Fagg, Duncan P.. Universidad de Aveiro; Portugal
Fil: Pérez Coll, Domingo. Instituto de Cerámica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; España
Fil: Mather, Glenn C.. Instituto de Cerámica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; España
Materia
Protonicos
Difraccion de Neutrones
SR-XRD
Fuel Cell
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:11336/99377
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/99377
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δHeras Juaristi, GemmaAmador, UlisesRomero de Paz, JulioFuentes, Rodolfo OscarChinelatto, Adilson L.Ritter, ClemensFagg, Duncan P.Pérez Coll, DomingoMather, Glenn C.ProtonicosDifraccion de NeutronesSR-XRDFuel Cellhttps://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2The BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ -BaPrO 3-δ perovskite system, of interest for high-temperature electrochemical applications involving mixed protonic-electronic conductivity, forms a solid-solution with a wide interval of Ba substoichiometry in the range Ba(Ce 0.2 Zr 0.7 ) 1-x Pr x Y 0.1 O 3-δ , 0 ≤ x ≤ 1. Structural phase transitions mapped as a function of temperature and composition by high-resolution neutron powder diffraction and synchrotron X-ray diffraction reveal higher symmetry for lower Pr content and higher temperatures, with the largest stability field observed for rhombohedral symmetry (space group, R3c). Rietveld refinement, supported by magnetic-susceptibility measurements, indicates that partitioning of the B-site cations over the A and B perovskite sites compensates Ba substoichiometry in preference to A-site vacancy formation and that multiple cations are distributed over both sites. Electron-hole transport dominates electrical conductivity in both wet and dry oxidizing conditions, with total conductivity reaching a value of 0.5 S cm -1 for the x = 1 end-member in dry air at 1173 K. Higher electrical conductivity and the displacement of oxygen loss to higher temperatures with increasing Pr content both reflect the role of Pr in promoting hole formation at the expense of oxygen vacancies. In more reducing conditions (N 2 ) and at low Pr contents, conductivity is higher in humidified atmospheres (0.023 atm pH 2 O) indicating a protonic contribution to transport, whereas the greater electron-hole conductivity with increasing Pr content results in lower conductivity in humidified N 2 due to the creation of protonic defects and the consumption of holes.Fil: Heras Juaristi, Gemma. Instituto de Ceramica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; EspañaFil: Amador, Ulises. Universidad CEU-San Pablo; EspañaFil: Romero de Paz, Julio. Universidad Complutense de Madrid; EspañaFil: Fuentes, Rodolfo Oscar. Comisión Nacional de Energía Atómica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Chinelatto, Adilson L.. Universidade Estadual de Ponta Grossa; BrasilFil: Ritter, Clemens. Institut Laue-Langevin; FranciaFil: Fagg, Duncan P.. Universidad de Aveiro; PortugalFil: Pérez Coll, Domingo. Instituto de Cerámica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; EspañaFil: Mather, Glenn C.. Instituto de Cerámica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; EspañaAmerican Chemical Society2018-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/99377Heras Juaristi, Gemma; Amador, Ulises; Romero de Paz, Julio; Fuentes, Rodolfo Oscar; Chinelatto, Adilson L.; et al.; Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ; American Chemical Society; Inorganic Chemistry; 57; 23; 12-2018; 15023-150330020-1669CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/acs.inorgchem.8b02956info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.inorgchem.8b02956info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:33:09Zoai:ri.conicet.gov.ar:11336/99377instacron: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:34982025-09-29 10:33:10.215CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
title Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
spellingShingle Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
Heras Juaristi, Gemma
Protonicos
Difraccion de Neutrones
SR-XRD
Fuel Cell
title_short Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
title_full Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
title_fullStr Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
title_full_unstemmed Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
title_sort Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ
dc.creator.none.fl_str_mv Heras Juaristi, Gemma
Amador, Ulises
Romero de Paz, Julio
Fuentes, Rodolfo Oscar
Chinelatto, Adilson L.
Ritter, Clemens
Fagg, Duncan P.
Pérez Coll, Domingo
Mather, Glenn C.
author Heras Juaristi, Gemma
author_facet Heras Juaristi, Gemma
Amador, Ulises
Romero de Paz, Julio
Fuentes, Rodolfo Oscar
Chinelatto, Adilson L.
Ritter, Clemens
Fagg, Duncan P.
Pérez Coll, Domingo
Mather, Glenn C.
author_role author
author2 Amador, Ulises
Romero de Paz, Julio
Fuentes, Rodolfo Oscar
Chinelatto, Adilson L.
Ritter, Clemens
Fagg, Duncan P.
Pérez Coll, Domingo
Mather, Glenn C.
author2_role author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Protonicos
Difraccion de Neutrones
SR-XRD
Fuel Cell
topic Protonicos
Difraccion de Neutrones
SR-XRD
Fuel Cell
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.5
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ -BaPrO 3-δ perovskite system, of interest for high-temperature electrochemical applications involving mixed protonic-electronic conductivity, forms a solid-solution with a wide interval of Ba substoichiometry in the range Ba(Ce 0.2 Zr 0.7 ) 1-x Pr x Y 0.1 O 3-δ , 0 ≤ x ≤ 1. Structural phase transitions mapped as a function of temperature and composition by high-resolution neutron powder diffraction and synchrotron X-ray diffraction reveal higher symmetry for lower Pr content and higher temperatures, with the largest stability field observed for rhombohedral symmetry (space group, R3c). Rietveld refinement, supported by magnetic-susceptibility measurements, indicates that partitioning of the B-site cations over the A and B perovskite sites compensates Ba substoichiometry in preference to A-site vacancy formation and that multiple cations are distributed over both sites. Electron-hole transport dominates electrical conductivity in both wet and dry oxidizing conditions, with total conductivity reaching a value of 0.5 S cm -1 for the x = 1 end-member in dry air at 1173 K. Higher electrical conductivity and the displacement of oxygen loss to higher temperatures with increasing Pr content both reflect the role of Pr in promoting hole formation at the expense of oxygen vacancies. In more reducing conditions (N 2 ) and at low Pr contents, conductivity is higher in humidified atmospheres (0.023 atm pH 2 O) indicating a protonic contribution to transport, whereas the greater electron-hole conductivity with increasing Pr content results in lower conductivity in humidified N 2 due to the creation of protonic defects and the consumption of holes.
Fil: Heras Juaristi, Gemma. Instituto de Ceramica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; España
Fil: Amador, Ulises. Universidad CEU-San Pablo; España
Fil: Romero de Paz, Julio. Universidad Complutense de Madrid; España
Fil: Fuentes, Rodolfo Oscar. Comisión Nacional de Energía Atómica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Chinelatto, Adilson L.. Universidade Estadual de Ponta Grossa; Brasil
Fil: Ritter, Clemens. Institut Laue-Langevin; Francia
Fil: Fagg, Duncan P.. Universidad de Aveiro; Portugal
Fil: Pérez Coll, Domingo. Instituto de Cerámica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; España
Fil: Mather, Glenn C.. Instituto de Cerámica y Vidrio de Madrid; España. Consejo Superior de Investigaciones Científicas; España
description The BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ -BaPrO 3-δ perovskite system, of interest for high-temperature electrochemical applications involving mixed protonic-electronic conductivity, forms a solid-solution with a wide interval of Ba substoichiometry in the range Ba(Ce 0.2 Zr 0.7 ) 1-x Pr x Y 0.1 O 3-δ , 0 ≤ x ≤ 1. Structural phase transitions mapped as a function of temperature and composition by high-resolution neutron powder diffraction and synchrotron X-ray diffraction reveal higher symmetry for lower Pr content and higher temperatures, with the largest stability field observed for rhombohedral symmetry (space group, R3c). Rietveld refinement, supported by magnetic-susceptibility measurements, indicates that partitioning of the B-site cations over the A and B perovskite sites compensates Ba substoichiometry in preference to A-site vacancy formation and that multiple cations are distributed over both sites. Electron-hole transport dominates electrical conductivity in both wet and dry oxidizing conditions, with total conductivity reaching a value of 0.5 S cm -1 for the x = 1 end-member in dry air at 1173 K. Higher electrical conductivity and the displacement of oxygen loss to higher temperatures with increasing Pr content both reflect the role of Pr in promoting hole formation at the expense of oxygen vacancies. In more reducing conditions (N 2 ) and at low Pr contents, conductivity is higher in humidified atmospheres (0.023 atm pH 2 O) indicating a protonic contribution to transport, whereas the greater electron-hole conductivity with increasing Pr content results in lower conductivity in humidified N 2 due to the creation of protonic defects and the consumption of holes.
publishDate 2018
dc.date.none.fl_str_mv 2018-12
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/11336/99377
Heras Juaristi, Gemma; Amador, Ulises; Romero de Paz, Julio; Fuentes, Rodolfo Oscar; Chinelatto, Adilson L.; et al.; Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ; American Chemical Society; Inorganic Chemistry; 57; 23; 12-2018; 15023-15033
0020-1669
CONICET Digital
CONICET
url http://hdl.handle.net/11336/99377
identifier_str_mv Heras Juaristi, Gemma; Amador, Ulises; Romero de Paz, Julio; Fuentes, Rodolfo Oscar; Chinelatto, Adilson L.; et al.; Structures, Phase Fields, and Mixed Protonic-Electronic Conductivity of Ba-Deficient, Pr-Substituted BaZr 0.7 Ce 0.2 Y 0.1 O 3-δ; American Chemical Society; Inorganic Chemistry; 57; 23; 12-2018; 15023-15033
0020-1669
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/acs.inorgchem.8b02956
info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.inorgchem.8b02956
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
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 13.070432

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