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

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'' ${\mathrm{CoSb}}_{3}$ 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.