Mg3Sb2-based Zintl compounds have garnered recent attention as promising materials for thermoelectric applications due to their low thermal conductivity and high zT values as n-type materials. However, the zT values of p-type materials are lower compared to their n-type counterparts. Through a straightforward process involving cold pressing and evacuating-and-encapsulating sintering, we have successfully synthesized a variety of p-type Mg3-xZnxSb2/Sb composites by adding the ZnSb-4%Sb composite into the Mg3Sb2 host material. Structural analyses have provided insights into the role of the ZnSb-4%Sb composite, demonstrating its significance in Zn doping on the Mg sites and Sb acting as an additive in the composite. The introduction of Zn on the Mg tetrahedral sites enhances the concentration of carriers, while the presence of highly conductive Sb grains facilitates the movement of charge carriers between adjacent Mg3-xZnxSb2 grains, thereby promoting mobility. Consequently, the electrical resistivity of the Mg3-xZnxSb2/Sb composites decreases as the Zn content increases. At 710 K, the Mg1.91Zn1.09Sb2/Sb composite exhibits the lowest resistivity, measuring 5.1 mΩ-cm, which is 46 times lower than that of the Mg3Sb2 host. Furthermore, the zT value of the Mg3-xZnxSb2/Sb composites increases with higher Zn content (x), benefiting from a combination of an improved power factor and reduced thermal conductivity. Significantly, our straightforward fabrication process enables us to achieve a maximum zT value of 0.58 at 710 K for the Mg1.91Zn1.09Sb2/Sb composite. This achievement can primarily be attributed to the 8-fold enhancement in power factor compared to the Mg3Sb2 host.
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