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Journal ArticleDOI

Effect of partial void filling on the lattice thermal conductivity of skutterudites

01 Jul 1998-Physical Review B (American Physical Society)-Vol. 58, Iss: 1, pp 164-170
TL;DR: Seebeck et al. as discussed by the authors measured the impact of partial void filling on the lattice thermal conductivity of polycrystalline antimonides with the skutterudite crystal structure with La partially filling the voids.
Abstract: Polycrystalline samples of antimonides with the skutterudite crystal structure with La partially filling the voids have been prepared in an effort to quantify the impact of partial void filling on the lattice thermal conductivity of these compounds. It is observed that a relatively small concentration of La in the voids results in a relatively large decrease in the lattice thermal conductivity. In addition, the largest decrease in the lattice thermal conductivity, compared to ‘‘unfilled’’ CoSb 3 is not observed near 100% filling of the voids with La, as was previously believed. This suggests a point-defect-type phonon scattering effect due to the partial, random distribution of La in the voids as well as the ‘‘rattling’’ effect of the La ions, resulting in the scattering of a larger spectrum of phonons than in the case of 100% filling. An additional benefit of partial filling in thermoelectric materials is that it may be one way of adjusting the electronic properties of these compounds. Seebeck, resistivity, Hall effect and structural data for these skutterudite compounds are also presented. @S0163-1829~98!02926-9#

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Journal ArticleDOI
TL;DR: The 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, and lattice thermal conductivity can also be significantly reduced, to values near the glass limit of these materials.
Abstract: Skutterudites CoSb3 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-fr...

1,222 citations

Journal ArticleDOI
TL;DR: In this paper, the authors proposed a method to compare one potential thermoelectric material with another, based on a numerical expression that is commonly used to compare the performance or efficiency of a particular device made from a material.
Abstract: ▪ Abstract Recently there has been a resurgence of research efforts related to the investigation of new and novel materials for small-scale thermoelectric refrigeration and power generation applications. These materials need to couple and optimize a variety of properties in order to exhibit the necessary figure of merit, i.e. the numerical expression that is commonly used to compare one potential thermoelectric material with another. The figure of merit is related to the coefficient of performance or efficiency of a particular device made from a material. The best thermoelectric material should possess thermal properties similar to that of a glass and electrical properties similar to that of a perfect single-crystal material, i.e. a poor thermal conductor and a good electrical conductor. Skutterudites are materials that appear to have the potential to fulfill such criteria. These materials exhibit many types of interesting properties. For example, skutterudites are members of a family of compounds we call...

827 citations

Journal ArticleDOI
TL;DR: In this paper, the synthesis process and the relationship between the microstructures and the thermoelectric properties of the nanostructured bulk materials with an enhanced ZT value are reviewed.
Abstract: Recently a significant figure-of-merit (ZT) improvement in the most-studied existing thermoelectric materials has been achieved by creating nanograins and nanostructures in the grains using the combination of high-energy ball milling and a direct-current-induced hot-press process. Thermoelectric transport measurements, coupled with microstructure studies and theoretical modeling, show that the ZT improvement is the result of low lattice thermal conductivity due to the increased phonon scattering by grain boundaries and structural defects. In this article, the synthesis process and the relationship between the microstructures and the thermoelectric properties of the nanostructured thermoelectric bulk materials with an enhanced ZT value are reviewed. It is expected that the nanostructured materials described here will be useful for a variety of applications such as waste heat recovery, solar energy conversion, and environmentally friendly refrigeration.

802 citations

Journal ArticleDOI
TL;DR: In this article, a polycrystalline skutterudite partially filled with ytterbium ions was shown to have a relatively high dimensionless figure of merit (ZT) in the presence of Yb atoms.
Abstract: We present evidence of a relatively high dimensionless figure of merit (ZT) in a polycrystalline skutterudite partially filled with ytterbium ions. The small-diameter yet heavy-mass Yb atoms partially filling the voids of the host CoSb3 system exhibit low values of thermal conductivity while the quite favorable electronic properties are not substantially perturbed by the addition of Yb. This combination is ideal for thermoelectric applications exemplifying the “phonon-glass electron-crystal” concept of a thermoelectric material, resulting in ZT=0.3 at room temperature and ZT∼1 at 600 K for Yb0.19Co4Sb12.

518 citations

Journal ArticleDOI
TL;DR: In this article, the lattice parameters increase linearly with Ba content, and the electrical conductivity increases with increasing the Ba filling fraction, reaching a maximum value of 1.1 for Ba0.24Co4Sb12 at 850 K.
Abstract: Barium-filled skutterudites BayCo4Sb12 with an anomalously large filling fraction of up to y=0.44 have been synthesized. The lattice parameters increase linearly with Ba content. Magnetic susceptibility data show that Ba0.44Co4Sb12 is paramagnetic, which implies that some of the Co atoms in BayCo4Sb12 have acquired a magnetic moment. The presence of the two different valence states of Co (Co3+ and Co2+) leads to the anomalously large barium filling fraction even without extra charge compensation. All samples show n-type conduction. The electrical conductivity increases with increasing the Ba filling fraction. The lattice thermal conductivity of BayCo4Sb12 is significantly depressed as compared to unfilled Co4Sb12. The dimensionless thermoelectric figure of merit, ZT, increases with increasing temperature reaching a maximum value of 1.1 for Ba0.24Co4Sb12 at 850 K.

393 citations