Substantial enhancement in thermoelectric figure-of-merit of half-Heusler ZrNiPb alloys

Ternary half-Heusler (HH) alloys are under intense investigations recently towards achieving high thermoelectric (TE) figure-of-merit (ZT). Of particular interest is the ZrNiPb-based HH alloy, where an optimal value of ZT ~ 0.7 at 773 K has been achieved by co-doping Sn and Bi at Pb site. In this work, we identify an excellent ZT of 1.3 in ZrNi_1+xPb_0.38Sn_0.6Bi_0.02 (x = 0.03, at 773 K) composite alloy. This is achieved by synergistic modulation of electronic as well as thermal properties via introduction of minor phase of full-Heusler (FH) in the HH matrix through compositional tuning approach. These Ni-rich ZrNi_1+xPb_0.38Sn_0.6Bi_0.02 (0 ≤ x ≤ 0.07) alloys were synthesized via energy efficient and time-curbed techniques that involved Arc melting followed by consolidation via spark plasma sintering. These alloys were characterized by XRD and SEM, which show formation of nanocomposites comprising of HH matrix phase and FH secondary minor phases. Enhancement in ZT is mainly attributed to a synchronized increase in power factor (~42%) and ~25% decrease in its thermal conductivity. Here, TE compatibility factor (S) was also calculated for all samples. The value of |S| ~ 2.7 V⁻¹ (at 773 K) is observed for x = 0.03, which is ~17% higher than bare HH composition (x = 0.0). The theoretically calculated TE device efficiency of best-performing sample ZrNi_1.03Pb_0.38Sn_0.6Bi_0.02 is estimated to be η ~ 13.6%. Our results imply that deliberately controlled fine tuning in compositions of HH compounds through compositional tuning approach would lead to novel off-stoichiometric HH phases with enhanced ZT value for efficient TE device fabrication.