Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics

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dc.contributor.authorSerrano Sánchez, F.
dc.contributor.authorPrado Gonjal, Jesús De La Paz
dc.contributor.authorNemes, Norbert Marcel
dc.contributor.authorBiskup Zaja, Nevenko
dc.contributor.authorDura, O. J.
dc.contributor.authorMartinez, J. L.
dc.contributor.authorFernandez Diaz, M. T.
dc.contributor.authorFauth, F.
dc.contributor.authorAlonso, J. A.
dc.date.accessioned2024-06-06T15:24:49Z
dc.date.available2024-06-06T15:24:49Z
dc.date.issued2018-09-28
dc.descriptionJuan de la Cierva fellowship FJCI-2015-2414
dc.description.abstractThe reduction of the lattice thermal conductivity is one of the crucial steps in improving thermoelectric materials. In skutterudites, a well-known approach is to reduce the thermal conductivity by filling the structural cage with rare-earth atoms. In this work, we show that it is not just the amount of such filling itself but its nanoscale structuration that lowers the thermal conductivity. A straightforward synthesis procedure under high pressure yields Ce- and Yb-filled CoSb3 skutterudites, with and without an inhomogeneous distribution of the filler atoms. The composition of the phases is evaluated from synchrotron Xray diffraction (SXRD) data; the highly nanostructured morphology is verified by high-resolution transmission electron microscopy (TEM). The filling fluctuation, i.e., the uneven distribution of filling atoms in the sample originating a phase segregation, brings about low lattice thermal conductivity, as a strong source of phonon scattering. This effect is prominent in the Ce-filled compound, where Ce is segregated into Ce-rich and Ce-poor regions, and the lattice contribution of the thermal conductivity kappa(L), shows a concomitant reduction, approaching values as low as 1.6 W m(-1) K-1 at 800 K. Although the level of filling is much higher in YbxCoSb3, its lattice thermal conductivity remains larger. Overall, though, its power factor is enhanced due to charge transfer from the Yb-filler. We thus define a new paradigm for the design of filled skutterudites with exceptionally low thermal conductivities, based on the nanoscale mixing of two phases with different filling factors, spontaneously induced by high-pressure synthesis conditions, which can be considered as pseudoamorphous structures with significant reduction in kappa(L).
dc.description.departmentDepto. de Física de Materiales
dc.description.departmentDepto. de Química Inorgánica
dc.description.facultyFac. de Ciencias Físicas
dc.description.facultyFac. de Ciencias Químicas
dc.description.facultyInstituto Pluridisciplinar (IP)
dc.description.refereedTRUE
dc.description.sponsorshipMinisterio de Economia y Competitividad (España)
dc.description.sponsorshipEuropean Commission
dc.description.sponsorshipMinisterio de Ciencia e Innovación (España)
dc.description.statuspub
dc.identifier.citationThermal Conductivity Reduction by Fluctuation of the Filling Fraction in Filled Cobalt Antimonide Skutterudite Thermoelectrics F. Serrano-Sánchez, J. Prado-Gonjal, N. M. Nemes, N. Biskup, O. J. Dura, J. L. Martínez, M. T. Fernández-Díaz, F. Fauth, and J. A. Alonso ACS Applied Energy Materials 2018 1 (11), 6181-6189 DOI: 10.1021/acsaem.8b01227
dc.identifier.doi10.1021/acsaem.8b01227
dc.identifier.essn2574-0962
dc.identifier.officialurlhttps://doi.org/10.1021/acsaem.8b01227
dc.identifier.relatedurlhttps://pubs.acs.org/doi/10.1021/acsaem.8b01227
dc.identifier.urihttps://hdl.handle.net/20.500.14352/104740
dc.issue.number11
dc.journal.titleACS Applied Energy Materials
dc.language.isoeng
dc.page.final6189
dc.page.initial6181
dc.publisherAmerican Chemical Society
dc.relation.projectIDinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/MAT2017-84496-R/ES/MATERIALES PARA CONVERSION DE ENERGIA: OXIDOS, CALCOGENUROS, PNICTUROS Y HALUROS/
dc.relation.projectIDinfo:eu-repo/grantAgreement/MINECO//MAT2014-52405-C2-2-R/ES/OPTIMIZACION DE PROPIEDADES ELECTRONICAS DE DISPOSITIVOS DE INTERFASE: SPIN-ORBITRONICA Y SPIN-MEMRISTORES/
dc.relation.projectIDinfo:eu-repo/grantAgreement/MINECO//MAT2015-66888-C3-3-R/ES/MAGNETISMO EN LA NANOESCALA: EXPLORANDO NUEVAS RUTAS (CRECIMIENTO Y CARACTERIZACION)/
dc.relation.projectID2017-T2/I ND-5597
dc.relation.projectIDinfo:eu-repo/grantAgreement/EC/H2020/713251/EU
dc.rights.accessRightsopen access
dc.subject.cdu538.9
dc.subject.cdu546
dc.subject.keywordFilling fraction fluctuation
dc.subject.keywordSkutterudites
dc.subject.keywordSynchrotron X-ray diffraction
dc.subject.keywordThermal conductivity
dc.subject.keywordThermoelectrics
dc.subject.ucmMateriales
dc.subject.ucmQuímica inorgánica (Química)
dc.subject.unesco2211 Física del Estado Sólido
dc.subject.unesco2303 Química Inorgánica
dc.titleThermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
dc.typejournal article
dc.type.hasVersionAM
dc.volume.number1
dspace.entity.typePublication
relation.isAuthorOfPublication7a2b8d3d-7159-48e6-a318-76923a9867ed
relation.isAuthorOfPublication697f3953-540b-435a-afc9-ec307315d667
relation.isAuthorOfPublication671e957a-9daa-4bd5-9876-eee854146782
relation.isAuthorOfPublication.latestForDiscovery7a2b8d3d-7159-48e6-a318-76923a9867ed
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