Thermoelectric Properties of Triple-Filled BaxYbyInzCo4Sb12 Skutterudites

Indium-filled skutterudites are promising power generation thermoelectric materials due to the presence of an InSb nanostructure that lowers the thermal conductivity. In this work, we have investigated thermoelectric properties of triple-filled Ba _x Yb _y In _z Co₄Sb₁₂ (0 ≤ x, y, z ≤ 0.14 actual) compounds by measuring their Seebeck coefficient, electrical conductivity, thermal conductivity, and Hall coefficient. All samples were prepared by a melting–annealing–spark plasma sintering method, and their structure was characterized by x-ray diffraction and transmission electron microscopy (TEM). TEM results show the development of an InSb nanostructure with a grain size of 30 nm to 500 nm. The nanostructure is present in all samples containing In and is also detected by specific heat measurements. The Seebeck and Hall coefficients indicate that the compounds are n-type semiconductors. Electrical conductivity increases with increasing Ba content. Thermal conductivity is strongly suppressed upon the presence of In in the skutterudite structure, likely due to enhanced boundary scattering of phonons on the nanometer-scale InSb inclusions. The highest thermoelectric figure of merit is achieved with Ba_0.09Yb_0.07In_0.06Co₄Sb_11.97, reaching ZT = 1.25 at 800 K.