Enhanced Thermoelectric and Mechanical Properties of ZrNiSn Half-Heusler Compounds by Excess Ag Doping at Ni Sites

Different from full-Heusler compounds, four vacancies in the face-centered cubic crystal structure provide extra sites for enhancing the thermoelectric properties of half-Heusler compounds (HHs). Herein, excess Ag is introduced to the Ni-site vacancies of ZrNiSn to optimize thermoelectric properties. The ZrNiAg_xSn (x = 0, 0.01, 0.02, and 0.03) samples were synthesized by levitation melting and spark plasma sintering. Remarkably, the introduction of excess Ag significantly improves the Seebeck coefficient of ZrNiAg_0.01Sn, and a peak power factor of ~ 4.52 mW/(m K²) is achieved in ZrNiAg_0.01Sn at 923 K, which is enhanced by 22.8% than that of pristine ZrNiSn. As a result, the figure of merit zT of pristine ZrNiSn is enhanced from ~ 0.60 to ~ 0.72 of ZrNiAg_0.01Sn at 923 K. Additionally, grain refinement effectively increases the Vickers hardness of ZrNiAg_0.01Sn, which is enhanced by 32.8% than that of pristine ZrNiSn. These results demonstrate a viable doping strategy for designing ZrNiSn-based HHs with excellent thermoelectric and mechanical properties.