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Thermoelectric properties of (GeTe)1-x[(Ag2Te)0.4(Sb2Te3)0.6]x alloys

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Abstract

The (GeTe)x(AgSbTe2)100-x alloys (TAGS-x) have been demonstrated as a promising p-type candidate for thermoelectric applications, attracting numerous attentions on the advancements of thermoelectric performance. Manipulation of carrier concentration for optimizing thermoelectric performance in TAGS can be achieved by varying the ratio of Ag to Sb, and the Ag/Sb ratio of ~ 2/3 has been proven as the optimal composition. Therefore, this work focuses on the systematic investigation on thermoelectric properties of (GeTe)1-x[(Ag2Te)0.4(Sb2Te3)0.6]x alloys. The crystal structure for the alloys transfers from rhombohedral to cubic at room temperature as x ≥ 0.2. The evolution of band parameter is estimated using a single parabolic band (SPB) model with acoustic phonon scattering. The density of states effective mass increases with x increasing, which leads to an enhancement of Seebeck coefficient along with a reduction in Hall mobility due to the additional carrier scattering by point defects. Meanwhile, the lattice thermal conductivity of lower than ~ 0.7 W·m−1·K−1 in the entire temperature range and the lowest one of only 0.45 W·m−1·K−1 is achieved due to additional phonon scattering by point defects. As a result, a peak thermoelectric figure of merit (zT) of ~ 1.80 and an average one of ~ 1.37 in 300–800 K are realized in nonstoichiometric TAGS alloys here.

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摘要

(GeTe)x(AgSbTe2)100-x合金 (TAGS-x) 是一种有前途的p型热电材料, 在热电性能提升方面引起了诸多关注。通过改变Ag与Sb的比例来调控载流子浓度可以优化TAGS的热电性能, 其中Ag/Sb的比例约为2/3被证实为最佳的组成。因此, 本工作对(GeTe)1-x[(Ag2Te)0.4(Sb2Te3)0.6]x合金的热电性能进行了系统研究。结果表明, 当x ≥ 0.2时, 样品的晶体结构在室温下从菱方结构转变为立方结构。利用基于声学声子散射的单抛物带 (SPB) 模型估计了材料的能带参数。态密度有效质量随着x的增加而增加, 从而导致了塞贝克系数的增加, 同时由于点缺陷造成的额外载流子散射导致霍尔迁移率降低。此外, 由于点缺陷引起的额外声子散射, 晶格热导率在整个温度范围内低于~0.7 W·m−1·K−1, 最低值仅为0.45 W·m−1·K−1。本工作在非化学计量的TAGS合金中实现的最高热电优值 (zT) 为~1.8, 在300-800 K 范围内的平均zT为~1.37。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 51861145305 and 52022068), the Fundamental Research Funds for Science and Technology Innovation Plan of Shanghai (No. 18JC1414600), Hefei National Laboratory for Physical Sciences at the Microscale (No. KF2020007) and Shanghai Natural Science Foundation (No. 19ZR1459900).

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  1. School of Materials Science and Engineering, Taiyuan University of Science and Technology, Taiyuan, 030024, China

    Hong-Xia Liu

  2. Laboratory of Magnetic and Electric Functional Materials and the Applications, The Key Laboratory of Shanxi Province, Taiyuan, 030024, China

    Hong-Xia Liu

  3. Interdisciplinary Materials Research Center, School of Materials Science and Engineering, Tongji University, Shanghai, 201804, China

    Hong-Xia Liu, Xin-Yue Zhang, Zhong-Lin Bu, Wen Li & Yan-Zhong Pei

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Liu, HX., Zhang, XY., Bu, ZL. et al. Thermoelectric properties of (GeTe)1-x[(Ag2Te)0.4(Sb2Te3)0.6]x alloys. Rare Met. 41, 921–930 (2022). https://doi.org/10.1007/s12598-021-01847-5

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