Enhancing the Thermoelectric Performance of n-Type Mg3.2Sb1.5Bi0.5 by Reducing Lattice Thermal Conductivity through the Incorporation of Chlorine-Containing Compounds

Mg3Sb2-based thermoelectric materials are characterized by their economic efficiency, nontoxicity, and environmental friendliness and represent a highly promising and eco-friendly functional material for midtemperature applications. To achieve a higher thermoelectric performance, we introduced two compounds, LaCl3 and CeCl3, into Mg3.2Sb1.5Bi0.5 under the guidance of first-principles calculations. The Mg3.2Sb1.5Bi0.5 + 0.03CeCl3 sample reached a maximum ZT value of approximately 1.6 at 723 K. The calculations indicate that two n-type dopants, LaCl3 and CeCl3, can adequately improve the band structure of Mg3Sb2, and the introduction of Cl atoms will also lead to lattice distortion and reduce the lattice thermal conductivity (κL). Experimental results demonstrate that the introduction of Cl atoms efficiently reduces the thermal conductivity while improving the electrical transport properties. Specifically, the Mg3.2Sb1.5Bi0.5 + 0.03CeCl3 sample achieved an exceptionally low κL of 0.3 W m–1 K–1 at 723 K, thereby validating the effectiveness of LaCl3 and CeCl3 doping. This work provides valuable insights into achieving thermoelectric decoupling in Mg3Sb2-based thermoelectric materials.