Computational Search for Better Thermoelectric Performance in Nickel-Based Half-Heusler Compounds

[Image: see text] Half-Heusler alloys have recently received extensive attention because of their promising thermoelectric (TE) properties and great potential for applications requiring efficient thermoelectricity. Although the conversion efficiency of these materials can be greatly improved by doping, it is still far away from the real-life applications. Therefore, search for better parent TE compounds is deemed urgent. Using a high-throughput search method based on first-principles calculations in newly proposed 378 half-Heusler alloys, we identify nine nickel-based half-Heusler semiconductors as candidates and systematically study their mechanical, electronic, and transport properties. Their mechanical and dynamical stabilities are verified based on the calculated elastic constants and phonon spectra. The electronic structure calculations indicate the existence of direct energy gaps in the NiVZ (Z = Al, Ga, and In) and indirect energy gaps in the NiTiZ (Z = Si, Ge, and Sn) and NiScZ (Z = P, As, and Sb) compounds. Among them, NiVAl, NiVGa, and NiVIn exhibit a sharp slope of density of states near the Fermi level, which is predicted to be essential for a high TE performance. Further investigation on carrier concentration and temperature dependence of TE properties shows the high power factors of NiVAl, NiVGa, and NiVIn, which are responsible for their high figure of merit values. The highest maximum power factor of 5.152 mW m(–1) K(–2) and figure of merit of 0.309 are predicted for pristine half-Heusler NiVIn, which are larger than the values of some known pristine and doped half-Heusler TE materials. Our work opens up new avenues for rationally searching better TE materials among half-Heusler alloys for applications in fields requiring efficient thermoelectricity.