Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution

Hybrid nanoparticles allow exploiting the interplay of confinement, proximity between different materials and interfacial effects. However, to harness their properties an in-depth understanding of their (meta)stability and interfacial characteristics is crucial. This is especially the case of nanosy...

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Autores: Roldan, Manuel A., Mayence, Arnaud, López-Ortega, Alberto|||0000-0003-3440-4444, Ishikawa, Ryo, Salafranca, Juan, Estrader i Bofarull, Marta|||0000-0003-3379-8234, Salazar Álvarez, Germán|||0000-0002-0671-435X, Baró, M. D.|||0000-0002-8636-1063, Nogués, Josep|||0000-0003-4616-1371, Pennycook, Stephen J., Varela del Arco, María|||0000-0002-6582-7004
Tipo de recurso: artículo
Fecha de publicación:2021
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:237749
Acceso en línea:https://ddd.uab.cat/record/237749
https://dx.doi.org/urn:doi:10.1016/j.cej.2020.126820
Access Level:acceso abierto
Palabra clave:Magnetic oxides
Core-shell nanoparticles
Scanning transmission electron microscopy
In-situ transformations
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spelling Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolutionRoldan, Manuel A.Mayence, ArnaudLópez-Ortega, Alberto|||0000-0003-3440-4444Ishikawa, RyoSalafranca, JuanEstrader i Bofarull, Marta|||0000-0003-3379-8234Salazar Álvarez, Germán|||0000-0002-0671-435XBaró, M. D.|||0000-0002-8636-1063Nogués, Josep|||0000-0003-4616-1371Pennycook, Stephen J.Varela del Arco, María|||0000-0002-6582-7004Magnetic oxidesCore-shell nanoparticlesScanning transmission electron microscopyIn-situ transformationsHybrid nanoparticles allow exploiting the interplay of confinement, proximity between different materials and interfacial effects. However, to harness their properties an in-depth understanding of their (meta)stability and interfacial characteristics is crucial. This is especially the case of nanosystems based on functional oxides working under reducing conditions, which may severely impact their properties. In this work, the in-situ electron-induced selective reduction of Mn₃O₄ to MnO is studied in magnetic Fe₃O₄/Mn₃O₄ and Mn₃O₄/Fe₃O₄ core/shell nanoparticles by means of high-resolution scanning transmission electron microscopy combined with electron energy-loss spectroscopy. Such in-situ transformation allows mimicking the actual processes in operando environments. A multi-stage image analysis using geometric phase analysis combined with particle image velocity enables direct monitoring of the relationship between structure, chemical composition and strain relaxation during the Mn₃O₄ reduction. In the case of Fe₃O₄/Mn₃O₄ core/shell the transformation occurs smoothly without the formation of defects. However, for the inverse Mn₃O₄/Fe₃O₄O core/shell configuration the electron beam-induced transformation occurs in different stages that include redox reactions and void formation followed by strain field relaxation via formation of defects. This study highlights the relevance of understanding the local dynamics responsible for changes in the particle composition in order to control stability and, ultimately, macroscopic functionality. 22021-01-0120212021-01-01Articlehttp://purl.org/coar/resource_type/c_6501SMURhttp://purl.org/coar/version/c_71e4c1898caa6e32info:eu-repo/semantics/articleapplication/pdfhttps://ddd.uab.cat/record/237749https://dx.doi.org/urn:doi:10.1016/j.cej.2020.126820reponame:Dipòsit Digital de Documents de la UABinstname:Universitat Autònoma de BarcelonaInglésengEuropean Commission https://doi.org/10.13039/501100000780 239739Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 IJCI-2014-21530Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 MAT2015-066888-C3-3-RAgencia Estatal de Investigación https://doi.org/10.13039/501100011033 MAT2016-77391-RMinisterio de Economía y Competitividad https://doi.org/10.13039/501100003329 SEV-2017-0706Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 RYC2018-024396-IAgencia Estatal de Investigación https://doi.org/10.13039/501100011033 RTI2018-097895-B-C43Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-292open accesshttp://purl.org/coar/access_right/c_abf2Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, i la comunicació pública de l'obra, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original. No es permet la creació d'obres derivades.https://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:ddd.uab.cat:2377492026-06-06T12:50:31Z
dc.title.none.fl_str_mv Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
title Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
spellingShingle Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
Roldan, Manuel A.
Magnetic oxides
Core-shell nanoparticles
Scanning transmission electron microscopy
In-situ transformations
title_short Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
title_full Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
title_fullStr Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
title_full_unstemmed Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
title_sort Probing the meta-stability of oxide core/shell nanoparticle systems at atomic resolution
dc.creator.none.fl_str_mv Roldan, Manuel A.
Mayence, Arnaud
López-Ortega, Alberto|||0000-0003-3440-4444
Ishikawa, Ryo
Salafranca, Juan
Estrader i Bofarull, Marta|||0000-0003-3379-8234
Salazar Álvarez, Germán|||0000-0002-0671-435X
Baró, M. D.|||0000-0002-8636-1063
Nogués, Josep|||0000-0003-4616-1371
Pennycook, Stephen J.
Varela del Arco, María|||0000-0002-6582-7004
author Roldan, Manuel A.
author_facet Roldan, Manuel A.
Mayence, Arnaud
López-Ortega, Alberto|||0000-0003-3440-4444
Ishikawa, Ryo
Salafranca, Juan
Estrader i Bofarull, Marta|||0000-0003-3379-8234
Salazar Álvarez, Germán|||0000-0002-0671-435X
Baró, M. D.|||0000-0002-8636-1063
Nogués, Josep|||0000-0003-4616-1371
Pennycook, Stephen J.
Varela del Arco, María|||0000-0002-6582-7004
author_role author
author2 Mayence, Arnaud
López-Ortega, Alberto|||0000-0003-3440-4444
Ishikawa, Ryo
Salafranca, Juan
Estrader i Bofarull, Marta|||0000-0003-3379-8234
Salazar Álvarez, Germán|||0000-0002-0671-435X
Baró, M. D.|||0000-0002-8636-1063
Nogués, Josep|||0000-0003-4616-1371
Pennycook, Stephen J.
Varela del Arco, María|||0000-0002-6582-7004
author2_role author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Magnetic oxides
Core-shell nanoparticles
Scanning transmission electron microscopy
In-situ transformations
topic Magnetic oxides
Core-shell nanoparticles
Scanning transmission electron microscopy
In-situ transformations
description Hybrid nanoparticles allow exploiting the interplay of confinement, proximity between different materials and interfacial effects. However, to harness their properties an in-depth understanding of their (meta)stability and interfacial characteristics is crucial. This is especially the case of nanosystems based on functional oxides working under reducing conditions, which may severely impact their properties. In this work, the in-situ electron-induced selective reduction of Mn₃O₄ to MnO is studied in magnetic Fe₃O₄/Mn₃O₄ and Mn₃O₄/Fe₃O₄ core/shell nanoparticles by means of high-resolution scanning transmission electron microscopy combined with electron energy-loss spectroscopy. Such in-situ transformation allows mimicking the actual processes in operando environments. A multi-stage image analysis using geometric phase analysis combined with particle image velocity enables direct monitoring of the relationship between structure, chemical composition and strain relaxation during the Mn₃O₄ reduction. In the case of Fe₃O₄/Mn₃O₄ core/shell the transformation occurs smoothly without the formation of defects. However, for the inverse Mn₃O₄/Fe₃O₄O core/shell configuration the electron beam-induced transformation occurs in different stages that include redox reactions and void formation followed by strain field relaxation via formation of defects. This study highlights the relevance of understanding the local dynamics responsible for changes in the particle composition in order to control stability and, ultimately, macroscopic functionality.
publishDate 2021
dc.date.none.fl_str_mv 2
2021-01-01
2021
2021-01-01
dc.type.none.fl_str_mv Article
http://purl.org/coar/resource_type/c_6501
SMUR
http://purl.org/coar/version/c_71e4c1898caa6e32
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://ddd.uab.cat/record/237749
https://dx.doi.org/urn:doi:10.1016/j.cej.2020.126820
url https://ddd.uab.cat/record/237749
https://dx.doi.org/urn:doi:10.1016/j.cej.2020.126820
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv European Commission https://doi.org/10.13039/501100000780 239739
Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 IJCI-2014-21530
Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 MAT2015-066888-C3-3-R
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 MAT2016-77391-R
Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 SEV-2017-0706
Ministerio de Economía y Competitividad https://doi.org/10.13039/501100003329 RYC2018-024396-I
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 RTI2018-097895-B-C43
Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2017/SGR-292
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://creativecommons.org/licenses/by-nc-nd/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
https://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:Dipòsit Digital de Documents de la UAB
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