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Luo, Zhong-Zhen; Cai, Songting; Hao, Shiqiang; Bailey, Trevor P; Xie, Hongyao; Slade, Tyler J; Liu, Yukun; Luo, Yubo; Chen, Zixuan; Xu, Jianwei; Luo, Wenjun; Yu, Yan; Uher, Ctirad; Wolverton, Christopher; Dravid, Vinayak P; Zou, Zhigang; Yan, Qingyu; Kanatzidis, Mercouri G
Journal of the American Chemical Society, 04/2022, Volume: 144, Issue: 16Journal Article
Converting waste heat into useful electricity using solid-state thermoelectrics has a potential for enormous global energy savings. Lead chalcogenides are among the most prominent thermoelectric materials, whose performance decreases with an increase in chalcogen amounts (e.g., PbTe > PbSe > PbS). Herein, we demonstrate the simultaneous optimization of the electrical and thermal transport properties of PbS-based compounds by alloying with GeS. The addition of GeS triggers a complex cascade of beneficial events as follows: Ge2+ substitution in Pb2+ and discordant off-center behavior; formation of Pb5Ge5S12 as stable second-phase inclusions through valence disproportionation of Ge2+ to Ge0 and Ge4+. PbS and Pb5Ge5S12 exhibit good conduction band energy alignment that preserves the high electron mobility; the formation of Pb5Ge5S12 increases the electron carrier concentration by introducing S vacancies. Sb doping as the electron donor produces a large power factor and low lattice thermal conductivity (κlat) of ∼0.61 W m–1 K–1. The highest performance was obtained for the 14% GeS-alloyed samples, which exhibited an increased room-temperature electron mobility of ∼121 cm2 V–1 s–1 for 3 × 1019 cm–3 carrier density and a ZT of 1.32 at 923 K. This is ∼55% greater than the corresponding Sb-doped PbS sample and is one of the highest reported for the n-type PbS system. Moreover, the average ZT (ZTavg) of ∼0.76 from 400 to 923 K is the highest for PbS-based systems.
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