Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites

[EN] Solid oxide electrochemical cells (SOCs) benefit from exsolution-based electrocatalyst design, where nanoparticles anchored in perovskites enhance stability and activity. Two of the most transformative features of this technology are the ability to engineer multielemental alloy nanoparticles fo...

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Autores: Delgado-Galicia, Blanca|||0009-0004-4655-5789, López-García, Andrés, Almar-Liante, Laura|||0000-0001-5103-3812, Carrillo-Del Teso, Alfonso Juan, Serra Alfaro, José Manuel|||0000-0002-1515-1106, Jimenez, Catalina Elena, Suarez-Anzorena, Rosario, Bar, Marcus, Perez-Dieste, Virginia, Aguadero, Ainara, Alonso, Jose A., Puente-Orench, Ines
Tipo de recurso: artículo
Fecha de publicación:2026
País:España
Institución:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:dnet:riunet______::6db82ffd09c1a00cbca09e5920206612
Acceso en línea:https://riunet.upv.es/handle/10251/235231
Access Level:acceso abierto
Palabra clave:Exsolution
Alloys
Janus nanoparticles
SOCs
Reversibility
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dc.title.none.fl_str_mv Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
title Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
spellingShingle Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
Delgado-Galicia, Blanca|||0009-0004-4655-5789
Exsolution
Alloys
Janus nanoparticles
SOCs
Reversibility
title_short Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
title_full Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
title_fullStr Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
title_full_unstemmed Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
title_sort Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex Perovskites
dc.creator.none.fl_str_mv Delgado-Galicia, Blanca|||0009-0004-4655-5789
López-García, Andrés
Almar-Liante, Laura|||0000-0001-5103-3812
Carrillo-Del Teso, Alfonso Juan
Serra Alfaro, José Manuel|||0000-0002-1515-1106
Jimenez, Catalina Elena
Suarez-Anzorena, Rosario
Bar, Marcus
Perez-Dieste, Virginia
Aguadero, Ainara
Alonso, Jose A.
Puente-Orench, Ines
author Delgado-Galicia, Blanca|||0009-0004-4655-5789
author_facet Delgado-Galicia, Blanca|||0009-0004-4655-5789
López-García, Andrés
Almar-Liante, Laura|||0000-0001-5103-3812
Carrillo-Del Teso, Alfonso Juan
Serra Alfaro, José Manuel|||0000-0002-1515-1106
Jimenez, Catalina Elena
Suarez-Anzorena, Rosario
Bar, Marcus
Perez-Dieste, Virginia
Aguadero, Ainara
Alonso, Jose A.
Puente-Orench, Ines
author_role author
author2 López-García, Andrés
Almar-Liante, Laura|||0000-0001-5103-3812
Carrillo-Del Teso, Alfonso Juan
Serra Alfaro, José Manuel|||0000-0002-1515-1106
Jimenez, Catalina Elena
Suarez-Anzorena, Rosario
Bar, Marcus
Perez-Dieste, Virginia
Aguadero, Ainara
Alonso, Jose A.
Puente-Orench, Ines
author2_role author
author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Instituto Universitario Mixto de Tecnología Química
Generalitat Valenciana
Agencia Estatal de Investigación
Bundesministerium für Bildung und Forschung, Alemania
Repositorio Institucional de la Universitat Politècnica de València Riunet
dc.subject.none.fl_str_mv Exsolution
Alloys
Janus nanoparticles
SOCs
Reversibility
topic Exsolution
Alloys
Janus nanoparticles
SOCs
Reversibility
description [EN] Solid oxide electrochemical cells (SOCs) benefit from exsolution-based electrocatalyst design, where nanoparticles anchored in perovskites enhance stability and activity. Two of the most transformative features of this technology are the ability to engineer multielemental alloy nanoparticles for tailored catalysis and the potential for in situ catalyst regeneration through redox-driven redissolution. However, the fundamental mechanisms governing these processes in complex, multicomponent systems remain poorly understood. In this work, the simultaneous exsolution of Fe, Ni, Co, and Cu from the fuel electrode material Sr2Fe1.2Co0.1Ni0.1Cu0.1Mo0.5O6-delta was investigated using in situ powder neutron diffraction and synchrotron-based near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS), combined with advanced electron microscopy to capture morphological evolution. At 700 degrees C, Cu-rich nanoparticles dominate, consistent with Ellingham reducibility trends; however, higher temperatures favor the formation of Fe-enriched alloys, driven by the high availability of Fe cations. Conversely, prolonged reduction promotes the formation of phase-separated Janus-type nanoparticles, primarily due to Fe-Cu immiscibility. Interestingly, redox cycling tests revealed that nanoparticle composition dictates redissolution capacity. While homogeneous alloys exhibited total redissolution into the perovskite backbone and subsequent re-exsolution, Janus-type nanoparticles underwent irreversible transformation into pyramidal NiO nanoparticles via intermediate cubic mixed oxide structures during air exposure. These findings elucidate how temperature, time, and elemental composition govern exsolved nanoparticle chemistry, morphology, and regeneration, establishing design principles for inducing multimetal exsolution in complex oxides toward enhanced electrocatalytic performance in energy conversion technologies.
publishDate 2026
dc.date.none.fl_str_mv 2026
2026-05-05
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://riunet.upv.es/handle/10251/235231
url https://riunet.upv.es/handle/10251/235231
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023 PID2022-139663OB-I00 DESCARBONIZACION DE LA INDUSTRIA DE PROCESOS MEDIANTE LA CATALISIS INTENSIFICADA POR INTEGRACION DE TECNOLOGIAS FACILITADORAS ESENCIALES
Bundesministerium für Bildung und Forschung, Alemania https://doi.org/10.13039/501100002347 FKZ 03EW0015B
Generalitat Valenciana https://doi.org/10.13039/501100003359 CIPROM%2F2022%2F10
Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 CEX2021-001230-S
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reconocimiento (by)
http://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Reconocimiento (by)
http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 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:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
instname:Universitat Politècnica de València (UPV)
instname_str Universitat Politècnica de València (UPV)
reponame_str RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
collection RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
repository.name.fl_str_mv
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spelling Impact of Phase-Separated Janus-Type Formation on the Reversibility of Multicomponent Exsolved Nanoparticles from Complex PerovskitesDelgado-Galicia, Blanca|||0009-0004-4655-5789López-García, AndrésAlmar-Liante, Laura|||0000-0001-5103-3812Carrillo-Del Teso, Alfonso JuanSerra Alfaro, José Manuel|||0000-0002-1515-1106Jimenez, Catalina ElenaSuarez-Anzorena, RosarioBar, MarcusPerez-Dieste, VirginiaAguadero, AinaraAlonso, Jose A.Puente-Orench, InesExsolutionAlloysJanus nanoparticlesSOCsReversibility[EN] Solid oxide electrochemical cells (SOCs) benefit from exsolution-based electrocatalyst design, where nanoparticles anchored in perovskites enhance stability and activity. Two of the most transformative features of this technology are the ability to engineer multielemental alloy nanoparticles for tailored catalysis and the potential for in situ catalyst regeneration through redox-driven redissolution. However, the fundamental mechanisms governing these processes in complex, multicomponent systems remain poorly understood. In this work, the simultaneous exsolution of Fe, Ni, Co, and Cu from the fuel electrode material Sr2Fe1.2Co0.1Ni0.1Cu0.1Mo0.5O6-delta was investigated using in situ powder neutron diffraction and synchrotron-based near-ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS), combined with advanced electron microscopy to capture morphological evolution. At 700 degrees C, Cu-rich nanoparticles dominate, consistent with Ellingham reducibility trends; however, higher temperatures favor the formation of Fe-enriched alloys, driven by the high availability of Fe cations. Conversely, prolonged reduction promotes the formation of phase-separated Janus-type nanoparticles, primarily due to Fe-Cu immiscibility. Interestingly, redox cycling tests revealed that nanoparticle composition dictates redissolution capacity. While homogeneous alloys exhibited total redissolution into the perovskite backbone and subsequent re-exsolution, Janus-type nanoparticles underwent irreversible transformation into pyramidal NiO nanoparticles via intermediate cubic mixed oxide structures during air exposure. These findings elucidate how temperature, time, and elemental composition govern exsolved nanoparticle chemistry, morphology, and regeneration, establishing design principles for inducing multimetal exsolution in complex oxides toward enhanced electrocatalytic performance in energy conversion technologies.Financial support by Generalitat Valenciana (CIPROM/2022/10) and by the Spanish Ministry of Science and Innovation (PID2022-139663OB-100 and CEX2021-001230-S) is gratefully acknowledged. These grants were funded by MCIN/AEI/10.13039/501100011033. We thank the financial support of the Helmholtz Initiative and Networking Fund through the German Federal Ministry of Education and Research (Bundesministerium fur Bildung und Forschung, BMBF) under Grant No. 03EW0015B (CatLab). These experiments were performed at BL24-CIRCE (proposal number 2024088545) beamlines at ALBA Synchrotron with the collaboration of ALBA staff. The authors wish to express their gratitude to the Institut Laue-Langevin (ILL) and the staff at D1B for making all facilities available for neutron diffraction experiments (Experiment No.CRG-2991). We thank the support of the Electronic Microscopy Service of the Universitat Politecnica de Valencia.American Chemical SocietyInstituto Universitario Mixto de Tecnología QuímicaGeneralitat ValencianaAgencia Estatal de InvestigaciónBundesministerium für Bildung und Forschung, AlemaniaRepositorio Institucional de la Universitat Politècnica de València Riunet20262026-05-05journal articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://riunet.upv.es/handle/10251/235231reponame:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valénciainstname:Universitat Politècnica de València (UPV)InglésengAgencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023 PID2022-139663OB-I00 DESCARBONIZACION DE LA INDUSTRIA DE PROCESOS MEDIANTE LA CATALISIS INTENSIFICADA POR INTEGRACION DE TECNOLOGIAS FACILITADORAS ESENCIALESBundesministerium für Bildung und Forschung, Alemania https://doi.org/10.13039/501100002347 FKZ 03EW0015BGeneralitat Valenciana https://doi.org/10.13039/501100003359 CIPROM%2F2022%2F10Agencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 CEX2021-001230-Sopen accesshttp://purl.org/coar/access_right/c_abf2Reconocimiento (by)http://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:dnet:riunet______::6db82ffd09c1a00cbca09e59202066122026-06-13T07:49:27Z
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