Thermoelectric Properties of N-type Mg<sub>3</sub>La<sub>0.005</sub>Mn<sub>x</sub>SbBi Materials Doped with La and Mn

Abstract

Mg<sub>3</sub>Sb<sub>2</sub>-based n-type materials are consisted of earth-abundant elements and possess comparable thermoelectric properties with n-type Bi<sub>2</sub>Te<sub>3</sub> at low temperatures, which make them promising candidates for cooling and power generation applications in terms of cost and performance. Substitution of Sb atom with chalcogen elements (Te, Se S) is a conventional method for n-type doping, but doping cations such as rare-earth elements and transition metals is also widely studied for its unique advantages. In this study, La and Mn were selected for co-doping of Mg3SbBi, and the thermoelectric performances of the doped materials were investigated. Mg<sub>3</sub>La<sub>0.005</sub>Mn<sub>x</sub>SbBi (0  <i>x</i>  0.015) polycrystalline samples were made by sintering the fine powders of the mother alloy after arc melting, in which elemental Mn and LaSb compound were included for n-type dual doping. Considering the loss of Mg at elevated temperatures by vaporization, the molar ratio of Mg, Sb, and Bi in the mixture for arc melting was set to 4 : 1 : 1 with excess Mg. Analysis shows that all the samples are n-type, and the electrical conductivity of Mg<sub>3</sub>La<sub>0.005</sub>Mn<sub>0.015</sub>SbBi increased by 62% from the Mn-free Mg<sub>3</sub>La<sub>0.005</sub>SbBi at 298 K. In addition, the lattice thermal conductivity (<i><sub>lat</sub></i>) decreased with increasing Mn content in the measured temperature range of 298-623 K. The minimum value of <i><sub>lat</sub></i> was about 0.60 W m<sup>-1</sup>K<sup>-1</sup> in Mg<sub>3</sub>La<sub>0.005</sub>Mn<sub>0.015</sub>SbBi at 523 K, which is about 19% smaller than that of the Mn-free sample. As a result of these enhancements in thermoelectric performance, the maximum figure of merit (<i>zT<sub>max</sub></i>) of 1.12 was obtained in Mg<sub>3</sub>La<sub>0.005</sub>Mn<sub>0.01</sub>SbBi and Mg<sub>3</sub>La<sub>0.005</sub>Mn<sub>0.015</sub>SbBi at 573 K, and the <i>zT</i> at 298 K increased by 73% to 0.35 in Mg<sub>3</sub>La<sub>0.005</sub>Mn<sub>0.015</sub>SbBi compared to Mn-free Mg<sub>3</sub>La<sub>0.005</sub>SbBi, which is beneficial to room-temperature applications.