Abstract
LiZnSb is a Zintl phase that has been predicted to be a good material in thermoelectric applications for a long time. However, experimental work indicated that the synthesized LiZnSb materials were p type, and their maximum zT value is only 0.08 at 525 K. CaZn0.4Ag0.2Sb, which belongs to the LiGaGe structure type and is also closely associated with the LiZnSb structure, did show high zT plateaus in a wide range of temperature, with the mixed transition metal Zn/Ag sites regulated. By comparing their crystallographic and electronic band structures, it is evident that the interlayered distances in both compounds have a great effect on the regulation of the corresponding electrical transport properties. When alloying CaZn0.4Ag0.2Sb with LiZnSb, solid solutions form within a specific range, which led to a marked enhancement in the Seebeck coefficient through the orbital alignment and carrier concentration optimization. In addition, a low thermal conductivity was obtained owing to the reduced electronic component. With the above optimization, a maximum zT value of ∼1.3 can be realized for (CaZn0.4Ag0.2Sb)0.87(LiZnSb)0.13 at 873 K, more than twice that of the pristine CaZn0.4Ag0.2Sb and about 10-fold compared to that of LiZnSb. This work may shed new light on the optimization of thermoelectric properties based on Zintl phases, for which the crystal structures are usually very complicated and a direct correlation between the structures and properties is difficult to make.
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