Synergistic effects of interstitial and substitutional doping on the thermoelectric properties of PbS

热电效应 兴奋剂 材料科学 热电材料 凝聚态物理 纳米技术 光电子学 热力学 物理
作者
Benteng Wu,Xueke Zhao,Mochen Jia,Dawei Yang,Yu Liu,Hongzhang Song,Dongyang Wang,Andreu Cabot,Mengyao Li
出处
期刊:Applied Physics Letters [American Institute of Physics]
卷期号:125 (22) 被引量:6
标识
DOI:10.1063/5.0238037
摘要

Lead sulfide (PbS) is widely recognized as a promising n-type thermoelectric material for use in the middle-temperature range. Although it already exhibits favorable electronic and thermal properties, its thermoelectric performance could be further enhanced by addressing the disparity between the light and heavy bands in the conduction band, thereby optimizing electrical transport, and by modifying the strength of its chemical bonds to reduce lattice thermal conductivity. In this study, we demonstrate that introducing just small amounts of antimony (Sb) into PbS generates a unique combination of interstitial and substitutional doping that leads to a significant improvement in both directions. Substitutional doping enhances the degeneracy between the light and heavy bands, increasing carrier mobility. At the same time, interstitial doping introduces a new resonance state near the Fermi level, providing an additional channel for electron transport while boosting carrier concentration. These synergistic effects lead to a marked increase in the power factor of PbS, achieving an average power factor (PFavg) of 1.07 mW m−1 K−2 across the temperature range of 320–873 K. Moreover, Sb substitution for Pb induces a shift in the surrounding S atoms toward Sb, weakening their bonds with neighboring Pb atoms. This shift results in a coexistence of strong and weak chemical bonds, which effectively reduces lattice thermal conductivity. Additionally, the defect structures introduced by Sb doping effectively scatter phonons, further lowering lattice thermal conductivity. As a result, PbS doped with 0.5% Sb exhibits a figure of merit (ZT) of 0.73 at 873 K, which is approximately three times higher than that of undoped PbS.
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