José Luis Martínez, Oscar J. Dura, François Fauth, José Antonio Alonso, Norbert M. Nemes, N. Biskup, Javier Gainza, Jesús Prado-Gonjal, Federico Serrano-Sánchez, Ministerio de Ciencia e Innovación (España), Comunidad de Madrid, European Research Council, European Commission, Universidad Complutense de Madrid, Consejo Superior de Investigaciones Científicas (España), Gainza, Javier [0000-0002-1999-3116], Serrano-Sánchez, Federico [0000-0002-6882-225X], Prado-Gonjal, Jesús [0000-0003-4880-8503], Nemes, Norbert Marce [0000-0002-7856-3642], Dura, O. J. [0000-0002-4014-7555], Martínez, J. L. [0000-0001-9046-8237], Fauth, Francois [0000-0001-9465-3106], Alonso, J. A. [0000-0001-5329-1225], Gainza, Javier, Serrano-Sánchez, Federico, Prado-Gonjal, Jesús, Nemes, Norbert Marce, Dura, O. J., Martínez, J. L., Fauth, Francois, and Alonso, J. A.
Thermoelectric mischmetal-filled MmxCo4Sb12 (Mm: natural cocktail of rare-earth elements, mostly Ce and La) skutterudites have been synthesized and sintered in one step under high-pressure conditions at 3.5 GPa in a piston–cylinder hydrostatic press. Synchrotron X-ray diffraction patterns display a splitting of the diffraction peaks ascribed to purely Ce-, and Mm-filled skutterudite phases, which have been analyzed and confirmed by high-resolution TEM and EELS. A total thermal conductivity (κ) of 1.51 W m−1 K−1 is measured at 773 K for Mm0.5Co4Sb12, below that of other filled skutterudites, which is promoted by the enhanced phonon scattering over a broad range of the phonon spectrum due to the inhomogeneous and nanoscale mischmetal inclusion. Compared to undoped CoSb3 skutterudite synthesized by conventional methods, κ is reduced by a factor of 3, while the power factor is also substantially enhanced., This work was supported by the Spanish Ministry of Science, Innovation and Universities through grants MAT2017-84496-R, MAT2017-87134-C2-2-R and MAT2015-66888-C3-3-R co financed by FEDER. JPG would also like to thank this Ministry for granting a “Juan de la Cierva” fellowship and to Community of Madrid for granting an “Atracción de Talento” fellowship (2017-T2/I ND-5597). Financial support from the ERC grant PoC2015-MAGTOOLS is also acknowledged. The authors wish to express their gratitude to ALBA technical staff for making the facilities available for the synchrotron X-ray diffraction experiment number 2017072260. Transmission electron microscopy studies were performed at the ICTS ELECMI node at Centro Nacional de Microscopía Electrónica (CNME) at the Universidad Complutense de Madrid (UCM)., We acknowledge support of the publication fee by the CSIC Open Access Support Initiative through its Unit of Information Resources for Research (URICI)