Realization of high thermoelectric performance in n-type partially filled skutterudites

Skutterudites are among the most exciting thermoelectric (TE) materials that could be used for various intermediate temperature applications. This study summarized our recent work on n-type partially filled skutterudites. By combining theoretical and experimental approaches, we revealed the underlying mechanism of void filling in the intrinsic lattice voids in CoSb3. With that, the electronegativity selection rule is established for the current stable filled skutterudites and further used for the discovery of a few novel filled CoSb3 compounds. The correlation between the thermal/electrical transport properties and impurity fillers in n-type partially filled skutterudites was also carefully investigated. Our results provide fundamental understanding to how those filler impurities affect electronic structures and lattice dynamics. Based on these basic understanding on transport mechanisms and sophisticated strategy in materials synthesis, TE figure of merit for n-type materials were continually increased from 1.1 to 1.4 and then to 1.7 for single-, double-, and triple-filled skutterudites.