title: Multiple-filled skutterudites: high thermoelectric figure of merit through separately optimizing electrical and thermal transports.
abstract: Skutterudites CoSb(3) with multiple cofillers Ba, La, and Yb were synthesized and very high thermoelectric figure of merit ZT = 1.7 at 850 K was realized. X-ray diffraction of the densified multiple-filled bulk samples reveals all samples are phase pure. High-resolution scanning transmission electron microscopy (STEM) and energy dispersive X-ray spectroscopy (EDS) analysis confirm that multiple guest fillers occupy the nanoscale-cages in the skutterudites. The fillers are further shown to be uniformly distributed and the Co-Sb skutterudite framework is virtually unperturbed from atomic scale to a few micrometers. Our results firmly show that high power factors can be realized by adjusting the total filling fraction of fillers with different charge states to reach the optimum carrier density, at the same time, lattice thermal conductivity can also be significantly reduced, to values near the glass limit of these materials, through combining filler species of different rattling frequencies to achieve broad-frequency phonon scattering. Therefore, partially filled skutterudites with multiple fillers of different chemical nature render unique structural characteristics for optimizing electrical and thermal transports in a relatively independent way, leading to continually enhanced ZT values from single- to double-, and finally to multiple-filled skutterudites. The idea of combining multiple fillers with different charge states and rattling frequencies for performance optimization is also expected to be valid for other caged TE compounds.
authors.affiliation: State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China.
authors.forename: Xun
authors.initials: X
authors.lastname: Shi
authors.forename: Jiong
authors.initials: J
authors.lastname: Yang
authors.forename: James R
authors.initials: JR
authors.lastname: Salvador
authors.forename: Miaofang
authors.initials: M
authors.lastname: Chi
authors.forename: Jung Y
authors.initials: JY
authors.lastname: Cho
authors.forename: Hsin
authors.initials: H
authors.lastname: Wang
authors.forename: Shengqiang
authors.initials: S
authors.lastname: Bai
authors.forename: Jihui
authors.initials: J
authors.lastname: Yang
authors.forename: Wenqing
authors.initials: W
authors.lastname: Zhang
authors.forename: Lidong
authors.initials: L
authors.lastname: Chen