A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles

Nanoparticles that combine several magnetic phases offer wide perspectives for cutting edge applications because of the high modularity of their magnetic properties. Besides the addition of the magnetic characteristics intrinsic to each phase, the interface that results from core–shell and, further,...

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Autores: Sartori, Kevin, Musat, Anamaria, Choueikani, Fadi, Grenèche, Jean Marc, Hettler, Simon, Bencok, Peter, Begin-Colin, Sylvie, Steadman, Paul, Arenal, Raúl, Pichon, Benoit P.
Formato: artículo
Estado:Versión enviada para evaluación y publicación
Fecha de publicación:2021
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/265427
Acesso em linha:http://hdl.handle.net/10261/265427
https://doi.org/10.1021/acsami.0c18310
Access Level:acceso abierto
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dc.title.none.fl_str_mv A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
title A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
spellingShingle A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
Sartori, Kevin
title_short A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
title_full A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
title_fullStr A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
title_full_unstemmed A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
title_sort A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticles
dc.creator.none.fl_str_mv Sartori, Kevin
Musat, Anamaria
Choueikani, Fadi
Grenèche, Jean Marc
Hettler, Simon
Bencok, Peter
Begin-Colin, Sylvie
Steadman, Paul
Arenal, Raúl
Pichon, Benoit P.
author Sartori, Kevin
author_facet Sartori, Kevin
Musat, Anamaria
Choueikani, Fadi
Grenèche, Jean Marc
Hettler, Simon
Bencok, Peter
Begin-Colin, Sylvie
Steadman, Paul
Arenal, Raúl
Pichon, Benoit P.
author_role author
author2 Musat, Anamaria
Choueikani, Fadi
Grenèche, Jean Marc
Hettler, Simon
Bencok, Peter
Begin-Colin, Sylvie
Steadman, Paul
Arenal, Raúl
Pichon, Benoit P.
author2_role author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Agence Nationale de la Recherche (France)
German Research Foundation
Ministerio de Economía y Competitividad (España)
Agencia Estatal de Investigación (España)
Ministerio de Ciencia, Innovación y Universidades (España)
European Commission
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
description Nanoparticles that combine several magnetic phases offer wide perspectives for cutting edge applications because of the high modularity of their magnetic properties. Besides the addition of the magnetic characteristics intrinsic to each phase, the interface that results from core–shell and, further, from onion structures leads to synergistic properties such as magnetic exchange coupling. Such a phenomenon is of high interest to overcome the superparamagnetic limit of iron oxide nanoparticles which hampers potential applications such as data storage or sensors. In this manuscript, we report on the design of nanoparticles with an onion-like structure which has been scarcely reported yet. These nanoparticles consist of a Fe3−δO4 core covered by a first shell of CoFe2O4 and a second shell of Fe3−δO4, e.g., a Fe3−δO4@CoFe2O4@Fe3−δO4 onion-like structure. They were synthesized through a multistep seed-mediated growth approach which consists consists in performing three successive thermal decomposition of metal complexes in a high-boiling-point solvent (about 300 °C). Although TEM micrographs clearly show the growth of each shell from the iron oxide core, core sizes and shell thicknesses markedly differ from what is suggested by the size increasing. We investigated very precisely the structure of nanoparticles in performing high resolution (scanning) TEM imaging and geometrical phase analysis (GPA). The chemical composition and spatial distribution of atoms were studied by electron energy loss spectroscopy (EELS) mapping and spectroscopy. The chemical environment and oxidation state of cations were investigated by 57Fe Mössbauer spectrometry, soft X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). The combination of these techniques allowed us to estimate the increase of Fe2+ content in the iron oxide core of the core@shell structure and the increase of the cobalt ferrite shell thickness in the core@shell@shell one, whereas the iron oxide shell appears to be much thinner than expected. Thus, the modification of the chemical composition as well as the size of the Fe3−δO4 core and the thickness of the cobalt ferrite shell have a high impact on the magnetic properties. Furthermore, the growth of the iron oxide shell also markedly modifies the magnetic properties of the core–shell nanoparticles, thus demonstrating the high potential of onion-like nanoparticles to accurately tune the magnetic properties of nanoparticles according to the desired applications.
publishDate 2021
dc.date.none.fl_str_mv 2021
2022
2022
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Preprint
info:eu-repo/semantics/submittedVersion
format article
status_str submittedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/265427
https://doi.org/10.1021/acsami.0c18310
url http://hdl.handle.net/10261/265427
https://doi.org/10.1021/acsami.0c18310
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
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info:eu-repo/grantAgreement/EC/H2020/823717
https://doi.org/10.1021/acsami.0c18310
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dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
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dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
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spelling A detailed investigation of the onion structure of exchanged coupled magnetic Fe3-δO4@CoFe2O4@Fe3-δO4 nanoparticlesSartori, KevinMusat, AnamariaChoueikani, FadiGrenèche, Jean MarcHettler, SimonBencok, PeterBegin-Colin, SylvieSteadman, PaulArenal, RaúlPichon, Benoit P.Nanoparticles that combine several magnetic phases offer wide perspectives for cutting edge applications because of the high modularity of their magnetic properties. Besides the addition of the magnetic characteristics intrinsic to each phase, the interface that results from core–shell and, further, from onion structures leads to synergistic properties such as magnetic exchange coupling. Such a phenomenon is of high interest to overcome the superparamagnetic limit of iron oxide nanoparticles which hampers potential applications such as data storage or sensors. In this manuscript, we report on the design of nanoparticles with an onion-like structure which has been scarcely reported yet. These nanoparticles consist of a Fe3−δO4 core covered by a first shell of CoFe2O4 and a second shell of Fe3−δO4, e.g., a Fe3−δO4@CoFe2O4@Fe3−δO4 onion-like structure. They were synthesized through a multistep seed-mediated growth approach which consists consists in performing three successive thermal decomposition of metal complexes in a high-boiling-point solvent (about 300 °C). Although TEM micrographs clearly show the growth of each shell from the iron oxide core, core sizes and shell thicknesses markedly differ from what is suggested by the size increasing. We investigated very precisely the structure of nanoparticles in performing high resolution (scanning) TEM imaging and geometrical phase analysis (GPA). The chemical composition and spatial distribution of atoms were studied by electron energy loss spectroscopy (EELS) mapping and spectroscopy. The chemical environment and oxidation state of cations were investigated by 57Fe Mössbauer spectrometry, soft X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). The combination of these techniques allowed us to estimate the increase of Fe2+ content in the iron oxide core of the core@shell structure and the increase of the cobalt ferrite shell thickness in the core@shell@shell one, whereas the iron oxide shell appears to be much thinner than expected. Thus, the modification of the chemical composition as well as the size of the Fe3−δO4 core and the thickness of the cobalt ferrite shell have a high impact on the magnetic properties. Furthermore, the growth of the iron oxide shell also markedly modifies the magnetic properties of the core–shell nanoparticles, thus demonstrating the high potential of onion-like nanoparticles to accurately tune the magnetic properties of nanoparticles according to the desired applications.K.S. was supported by a PhD grant from the French Agence Nationale de la Recherche (ANR) under the reference ANR11-LABX-0058-NIE within the Investissement d’Avenir program ANR-10-IDEX-0002-02 and SOLEIL synchrotron/Laboratoire Léon Brillouin fellowship. The authors are grateful to SOLEIL synchrotron light source for providing the access to DEIMOS beamline and to DIAMOND synchrotron light source for providing access to BLADE beamline. HRSTEM and STEM-EELS studies were conducted at the Laboratorio de Microscopias Avanzadas, Universidad de Zaragoza, Spain. S.H. is grateful to DFG (HE 7675/1-1). R.A. gratefully acknowledges the support from the Spanish Ministry of Economy and Competitiveness (MINECO) and the MICINN through project grants MAT2016-79776-P (AEI/FEDER, UE) and PID2019-104739GB-100/AEI/10.13039/501100011033 as well as from the European Union H2020 program “ESTEEM3” (823717).Peer reviewedAmerican Chemical SocietyAgence Nationale de la Recherche (France)German Research FoundationMinisterio de Economía y Competitividad (España)Agencia Estatal de Investigación (España)Ministerio de Ciencia, Innovación y Universidades (España)European CommissionConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202220222021info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Preprintinfo:eu-repo/semantics/submittedVersionhttp://hdl.handle.net/10261/265427https://doi.org/10.1021/acsami.0c18310reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/MINECO//MAT2016-79776-Pinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-104739GB-I00info:eu-repo/grantAgreement/EC/H2020/823717https://doi.org/10.1021/acsami.0c18310Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2654272026-05-22T06:33:51Z
score 15.81155

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