Significantly Enhanced Thermoelectric Performance of p-Type Mg3Sb2 via Zn Substitution on Mg(2) Site: Optimization of Hole Concentration Through Ag Doping

n-Type Mg3Sb2-based thermoelectric materials have recently garnered significant interest due to their superior thermoelectric efficiency. Yet, the advancement of p-type Mg3Sb2 for thermoelectric applications is impeded by its lower dimensionless figure of merit (zT). In this study, we demonstrate the improved thermoelectric performance of p-type Mg3Sb2 through the strategic optimization of Zn content and Ag doping on the Mg/Zn(2) site. Initially, samples of Mg3-xZnxSb2 (x = 0, 0.5, 1.0, and 1.5) were synthesized via elemental reactions within a Pyrex tube, followed by densification through hot pressing. X-ray diffraction analysis confirmed that the Mg3-xZnxSb2 phases retain the same P 3 m1 space group as the pristine Mg3Sb2 phase. The strategic substitution of Zn improved the power factor via band convergence and reduced lattice thermal conductivity by introducing point defect phonon scattering. This led to a peak zT of 0.5 at 725 K, with an average zT of 0.25 across the 325-725 K range. Enhancement in carrier concentration was achieved by doping Ag onto the Zn site, culminating in a peak zT of 0.95 at 725 K and an average zT of 0.46 between 325 and 725 K for the Mg2Zn0.97Ag0.03Sb2 sample. This performance surpasses that of most p-type Mg3Sb2-based materials, markedly advancing the potential for Mg3Sb2-based materials in midtemperature heat recovery thermoelectric generators.