The ZrNiSn-based half-Heusler compounds are promising for thermoelectric applications in the mid-to-high temperature range. However, their thermoelectric performance was greatly limited due to the remaining high thermal conductivity, especially the lattice thermal conductivity. Herein, we report the synthesis of pristine half-Heusler ZrNiSn through direct mechanical alloying at a liquid nitrogen temperature (i.e., cryomilling) followed by spark plasma sintering. It is shown that the onset sintering temperature is greatly reduced for the cryomilled powders with a high density. A reduced thermal conductivity is subsequently realized from room temperature to 700 °C in the cryomilled samples than the one that was differently prepared (from 7.3 to 4.5 W/m K at room temperature). The pronounced reduction in thermal conductivity of ZrNiSn yields a maximum zT of ∼0.65 at 700 °C. Our study shows the possibility of cryomilling in advancing the thermoelectric performance through enhanced phonon scattering.
Keywords: cryomilling; half-Heusler compounds; lattice thermal conductivity; spark plasma sintering.