Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks

We present the synthesis and magneto-thermal properties of carborane-based lanthanide metal-organic frameworks (MOFs) with the formula {[(Ln)3(mCB-L)4(NO3)(DMF)n]·Solv}, where Ln = Dy or Tb, characterized by dc and ac susceptibility, X-ray absorption spectroscopy (XAS), X-ray magnetic circular dichr...

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Autores: Li, Zhen, Arauzo, Ana B., Giner Planas, José, Bartolomé, Elena
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/364909
Acceso en línea:http://hdl.handle.net/10261/364909
https://api.elsevier.com/content/abstract/scopus_id/85191383979
Access Level:acceso abierto
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spelling Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworksLi, ZhenArauzo, Ana B.Giner Planas, JoséBartolomé, ElenaWe present the synthesis and magneto-thermal properties of carborane-based lanthanide metal-organic frameworks (MOFs) with the formula {[(Ln)3(mCB-L)4(NO3)(DMF)n]·Solv}, where Ln = Dy or Tb, characterized by dc and ac susceptibility, X-ray absorption spectroscopy (XAS), X-ray magnetic circular dichroism (XMCD) and heat capacity measurements. The MOF structure is formed by polymeric 1D chains of Ln ions with three different coordination environments (Ln1, Ln2, Ln3) running along the b-axis, linked by carborane-based linkers thus to provide a 3D structure. Static magnetic measurements reveal that these MOFs behave at low temperature as a system of S* = 1/2 Ising spins, weakly interacting ferromagnetically along the 1D polymeric chain (J*/kB = +0.45 K (+0.5 K) interaction constant estimated for Dy-MOF (Tb-MOF)) and coupled to Ln ions in adjacent chains through dipolar antiferromagnetic interactions. The Dy MOF exhibits slow relaxation of magnetization through a thermally activated process, transitioning to quantum tunneling of the magnetization at low temperatures, while both compounds exhibit field-induced relaxation through a very slow, direct process. The maximum magnetic entropy changes (-ΔSmaxm) for an applied magnetic field change of 2-0 T are 5.71 J kg-1 K-1 and 4.78 J kg-1 K-1, for Dy and Tb MOFs, respectively, while the magnetocaloric effect (MCE) peak for both occurs at T ∼ 1.6 K, approximately double that for the Gd counterpart.This work was financially supported by the Spanish Ministerio de Ciencia e Innovación projects PID2022-138492NB-I00 and PID2022-136892NB-I00, the Generalitat de Catalunya (2021/SGR/00442), and the Gobierno de Aragón (project RASMIA E12-23R). Zhen Li acknowledges the China Scholarship Council (CSC) for his PhD grant (201808310071). The authors would like to acknowledge the use of Servicio General de Apoyo a la Investigación-SAI, Universidad de Zaragoza. XAS and XMCD experiments were performed at the BOREAS beamline of the ALBA synchrotron with the support of ALBA staff (experiment number 2022085925).With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).Peer reviewedRoyal Society of Chemistry (UK)Ministerio de Ciencia e Innovación (España)Agencia Estatal de Investigación (España)Generalitat de CatalunyaGobierno de AragónChina Scholarship CouncilMinisterio de Ciencia, Innovación y Universidades (España)Li, Zhen [0000-0002-8497-7497]Arauzo, Ana [0000-0002-5999-341X]Giner Planas, José [0000-0002-1648-2169]Bartolomé, Elena [0000-0001-5108-0977]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202420242024info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10261/364909https://api.elsevier.com/content/abstract/scopus_id/85191383979reponame: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/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-138492NB-I00info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-136892NB-I00info:eu-repo/grantAgreement/AEI/Plan Estatal de investigación Científica y Técnica y de Innovación 2017-2020/CEX2019-000917-SDalton transactions (Cambridge, England : 2003)The underlying dataset has been published as supplementary material of the article in the publisher platform at DOI 10.1039/D4DT00626Ghttp://doi.org/10.1039/d4dt00626gSíinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3649092026-05-22T06:33:51Z
dc.title.none.fl_str_mv Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
title Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
spellingShingle Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
Li, Zhen
title_short Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
title_full Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
title_fullStr Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
title_full_unstemmed Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
title_sort Magnetic properties and magnetocaloric effect of Ln = Dy, Tb carborane-based metal-organic frameworks
dc.creator.none.fl_str_mv Li, Zhen
Arauzo, Ana B.
Giner Planas, José
Bartolomé, Elena
author Li, Zhen
author_facet Li, Zhen
Arauzo, Ana B.
Giner Planas, José
Bartolomé, Elena
author_role author
author2 Arauzo, Ana B.
Giner Planas, José
Bartolomé, Elena
author2_role author
author
author
dc.contributor.none.fl_str_mv Ministerio de Ciencia e Innovación (España)
Agencia Estatal de Investigación (España)
Generalitat de Catalunya
Gobierno de Aragón
China Scholarship Council
Ministerio de Ciencia, Innovación y Universidades (España)
Li, Zhen [0000-0002-8497-7497]
Arauzo, Ana [0000-0002-5999-341X]
Giner Planas, José [0000-0002-1648-2169]
Bartolomé, Elena [0000-0001-5108-0977]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
description We present the synthesis and magneto-thermal properties of carborane-based lanthanide metal-organic frameworks (MOFs) with the formula {[(Ln)3(mCB-L)4(NO3)(DMF)n]·Solv}, where Ln = Dy or Tb, characterized by dc and ac susceptibility, X-ray absorption spectroscopy (XAS), X-ray magnetic circular dichroism (XMCD) and heat capacity measurements. The MOF structure is formed by polymeric 1D chains of Ln ions with three different coordination environments (Ln1, Ln2, Ln3) running along the b-axis, linked by carborane-based linkers thus to provide a 3D structure. Static magnetic measurements reveal that these MOFs behave at low temperature as a system of S* = 1/2 Ising spins, weakly interacting ferromagnetically along the 1D polymeric chain (J*/kB = +0.45 K (+0.5 K) interaction constant estimated for Dy-MOF (Tb-MOF)) and coupled to Ln ions in adjacent chains through dipolar antiferromagnetic interactions. The Dy MOF exhibits slow relaxation of magnetization through a thermally activated process, transitioning to quantum tunneling of the magnetization at low temperatures, while both compounds exhibit field-induced relaxation through a very slow, direct process. The maximum magnetic entropy changes (-ΔSmaxm) for an applied magnetic field change of 2-0 T are 5.71 J kg-1 K-1 and 4.78 J kg-1 K-1, for Dy and Tb MOFs, respectively, while the magnetocaloric effect (MCE) peak for both occurs at T ∼ 1.6 K, approximately double that for the Gd counterpart.
publishDate 2024
dc.date.none.fl_str_mv 2024
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/364909
https://api.elsevier.com/content/abstract/scopus_id/85191383979
url http://hdl.handle.net/10261/364909
https://api.elsevier.com/content/abstract/scopus_id/85191383979
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
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info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-138492NB-I00
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2022-136892NB-I00
info:eu-repo/grantAgreement/AEI/Plan Estatal de investigación Científica y Técnica y de Innovación 2017-2020/CEX2019-000917-S
Dalton transactions (Cambridge, England : 2003)
The underlying dataset has been published as supplementary material of the article in the publisher platform at DOI 10.1039/D4DT00626G
http://doi.org/10.1039/d4dt00626g
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
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dc.publisher.none.fl_str_mv Royal Society of Chemistry (UK)
publisher.none.fl_str_mv Royal Society of Chemistry (UK)
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