Grain boundary engineering with nano-scale InSb producing high performance InxCeyCo4Sb12+z skutterudite thermoelectrics

Abstract

Thermoelectric semiconductors based on CoSb3 hold the best promise for recovering industrial or automotive waste heat because of their high efficiency and relatively abundant, lead-free constituent elements. However, higher efficiency is needed before thermoelectrics reach economic viability for widespread use. In this study, n-type InxCeyCo4Sb12+z skutterudites with high thermoelectric performance are produced by combining several phonon scattering mechanisms in a panoscopic synthesis. Using melt spinning followed by spark plasma sintering (MS-SPS), bulk InxCeyCo4Sb12+z alloys are formed with grain boundaries decorated with nano-phase of InSb. The skutterudite matrix has grains on a scale of 100-200 nm and the InSb nano-phase with a typical size of 5-15 nm is evenly dispersed at the grain boundaries of the skutterudite matrix. Coupled with the presence of defects on the Sb sublattice, this multi-scale nanometer structure is exceptionally effective in scattering phonons and, therefore, InxCeyCo4Sb12/InSb nano-composites have very low lattice thermal conductivity and high zT values reaching in excess of 1.5 at 800 K.