Neutron diffraction and thermoelectric properties of indium filled In_xCo₄Sb₁₂ (x = 0.05, 0.2) and indium cerium filled Ce_0.05In_0.1Co₄Sb₁₂ skutterudites

The thermoelectric properties on polycrystalline single (In) and double filled (Ce, In) skutterudites are characterized between 300 and 700 K. Powder neutron diffraction measurements of the skutterudite compositions In_xCo₄Sb₁₂ (x = 0.05, 0.2) and Ce_0.05In_0.1Co₄Sb₁₂ as a function of temperature (12-300 K) were carried out, which gives more insight into the structural data of single and double-filled skutterudites. Results show that due to the annealing treatment, a Sb deficiency is detectable and thus verifies defects at the Sb lattice site of the skutterudite. Furthermore, we show by electron microprobe analysis that a considerable amount of indium is lost during synthesis and post-processing for the single indium filled samples, but not for the double cerium and indium skutterudite sample. In our experiments, the double-filled skutterudite is superior to the single-filled skutterudite composition due to a higher charge carrier density, a comparable lattice thermal resistivity, and a higher density of states effective mass. Furthermore, we obtained a significantly higher Einstein temperature for the double-filled skutterudite composition in comparison to the single-filled species, which reflects the high sensitivity due to filling of the void lattice position within the skutterudite crystal.