Achieving High Thermoelectric Performance of Eco-Friendly SnTe-Based Materials by Selective Alloying and Defect Modulation.

Recently, rock-salt lead-free chalcogenide SnTe-based thermoelectric (TE) materials have been considered an alternative to PbTe because of the nontoxic properties of Sn as compared to Pb. However, high carrier concentration that originated from intrinsic Sn vacancies and relatively high thermal conductivity of pristine SnTe lead to poor TE efficiency, which makes room for improving its TE properties. In this study, we present that the Na incorporation into the SnTe matrix is helpful for modifying the electronic band structure, optimization of carrier concentration, introducing dislocations, and kink planes; benefiting from these synergistic effects obviates the disadvantages of SnTe and makes a significant improvement in TE performance. We reveal that Na favorably impacts the structure of electronic bands by valence, conduction band engineering, leading to a nice enhancement in the Seebeck coefficient, which exhibits the highest power factor value of 37.93 μWcm -1 K -2 at 898 K, representing the best result for the SnTe material system. Moreover, a broader phonon spectrum is introduced by new phonon-scattering centers, scattered by dislocations and kink planes which suppressed lattice thermal conductivity to 0.57 Wm -1 K -1 at 898 K, which is much lower than that of pristine SnTe. Ultimately, a maximum ZT of 1.26 at 898 K is achieved in the Sn 1.03 Te + 3% Na sample, which is 97% higher than that of the pristine SnTe, suggesting that SnTe-based materials are a robust candidate for TE applications specifically, an ideal alternative of lead chalcogenides for TE power generation at high temperatures.