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

The 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 amoun...

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Autores: Serrano Sánchez, F., Prado Gonjal, Jesús de la Paz, Nemes, Norbert Marcel, Biskup Zaja, Nevenko, Dura, O. J., Martinez, J. L., Fernandez Diaz, M. T., Fauth, F., Alonso, J. A.
Formato: artículo
Fecha de publicación:2018
País:España
Recursos:Universidad Complutense de Madrid (UCM)
Repositorio:Docta Complutense
Idioma:inglés
OAI Identifier:oai:docta.ucm.es:20.500.14352/104740
Acesso em linha:https://hdl.handle.net/20.500.14352/104740
Access Level:acceso abierto
Palavra-chave:538.9
546
Filling fraction fluctuation
Skutterudites
Synchrotron X-ray diffraction
Thermal conductivity
Thermoelectrics
Materiales
Química inorgánica (Química)
2211 Física del Estado Sólido
2303 Química Inorgánica
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oai_identifier_str oai:docta.ucm.es:20.500.14352/104740
network_acronym_str ES
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repository_id_str
spelling Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectricsSerrano Sánchez, F.Prado Gonjal, Jesús de la PazNemes, Norbert MarcelBiskup Zaja, NevenkoDura, O. J.Martinez, J. L.Fernandez Diaz, M. T.Fauth, F.Alonso, J. A.538.9546Filling fraction fluctuationSkutteruditesSynchrotron X-ray diffractionThermal conductivityThermoelectricsMaterialesQuímica inorgánica (Química)2211 Física del Estado Sólido2303 Química InorgánicaThe 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).American Chemical SocietyUniversidad Complutense de Madrid20182018-09-2820182018-09-28journal articlehttp://purl.org/coar/resource_type/c_6501AMhttp://purl.org/coar/version/c_ab4af688f83e57aainfo:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/20.500.14352/104740reponame:Docta Complutenseinstname:Universidad Complutense de Madrid (UCM)InglésengAgencia Estatal de Investigación http://dx.doi.org/10.13039/501100011033 Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016 MAT2017-84496-R MATERIALES PARA CONVERSION DE ENERGIA: OXIDOS, CALCOGENUROS, PNICTUROS Y HALUROSMinisterio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 Not available MAT2014-52405-C2-2-R OPTIMIZACION DE PROPIEDADES ELECTRONICAS DE DISPOSITIVOS DE INTERFASE: SPIN-ORBITRONICA Y SPIN-MEMRISTORESMinisterio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 Not available MAT2015-66888-C3-3-R MAGNETISMO EN LA NANOESCALA: EXPLORANDO NUEVAS RUTAS (CRECIMIENTO Y CARACTERIZACION)European Commission http://dx.doi.org/10.13039/501100000780 Horizon 2020 Framework Programme 713251open accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:docta.ucm.es:20.500.14352/1047402026-06-02T12:44:21Z
dc.title.none.fl_str_mv Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
title Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
spellingShingle Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
Serrano Sánchez, F.
538.9
546
Filling fraction fluctuation
Skutterudites
Synchrotron X-ray diffraction
Thermal conductivity
Thermoelectrics
Materiales
Química inorgánica (Química)
2211 Física del Estado Sólido
2303 Química Inorgánica
title_short Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
title_full Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
title_fullStr Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
title_full_unstemmed Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
title_sort Thermal conductivity reduction by fluctuation of the filling fraction in filled cobalt antimonide skutterudite thermoelectrics
dc.creator.none.fl_str_mv Serrano Sánchez, F.
Prado Gonjal, Jesús de la Paz
Nemes, Norbert Marcel
Biskup Zaja, Nevenko
Dura, O. J.
Martinez, J. L.
Fernandez Diaz, M. T.
Fauth, F.
Alonso, J. A.
author Serrano Sánchez, F.
author_facet Serrano Sánchez, F.
Prado Gonjal, Jesús de la Paz
Nemes, Norbert Marcel
Biskup Zaja, Nevenko
Dura, O. J.
Martinez, J. L.
Fernandez Diaz, M. T.
Fauth, F.
Alonso, J. A.
author_role author
author2 Prado Gonjal, Jesús de la Paz
Nemes, Norbert Marcel
Biskup Zaja, Nevenko
Dura, O. J.
Martinez, J. L.
Fernandez Diaz, M. T.
Fauth, F.
Alonso, J. A.
author2_role author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Universidad Complutense de Madrid
dc.subject.none.fl_str_mv 538.9
546
Filling fraction fluctuation
Skutterudites
Synchrotron X-ray diffraction
Thermal conductivity
Thermoelectrics
Materiales
Química inorgánica (Química)
2211 Física del Estado Sólido
2303 Química Inorgánica
topic 538.9
546
Filling fraction fluctuation
Skutterudites
Synchrotron X-ray diffraction
Thermal conductivity
Thermoelectrics
Materiales
Química inorgánica (Química)
2211 Física del Estado Sólido
2303 Química Inorgánica
description The 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).
publishDate 2018
dc.date.none.fl_str_mv 2018
2018-09-28
2018
2018-09-28
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
AM
http://purl.org/coar/version/c_ab4af688f83e57aa
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/20.500.14352/104740
url https://hdl.handle.net/20.500.14352/104740
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 2013-2016 MAT2017-84496-R MATERIALES PARA CONVERSION DE ENERGIA: OXIDOS, CALCOGENUROS, PNICTUROS Y HALUROS
Ministerio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 Not available MAT2014-52405-C2-2-R OPTIMIZACION DE PROPIEDADES ELECTRONICAS DE DISPOSITIVOS DE INTERFASE: SPIN-ORBITRONICA Y SPIN-MEMRISTORES
Ministerio de Economía y Competitividad http://dx.doi.org/10.13039/501100003329 Not available MAT2015-66888-C3-3-R MAGNETISMO EN LA NANOESCALA: EXPLORANDO NUEVAS RUTAS (CRECIMIENTO Y CARACTERIZACION)
European Commission http://dx.doi.org/10.13039/501100000780 Horizon 2020 Framework Programme 713251
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
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
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:Docta Complutense
instname:Universidad Complutense de Madrid (UCM)
instname_str Universidad Complutense de Madrid (UCM)
reponame_str Docta Complutense
collection Docta Complutense
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.300719

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