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Achieving high carrier mobility and low lattice thermal conductivity in GeTe-based alloys by cationic/anionic co-doping

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Abstract

The IV–VI compound GeTe is considered as a promising alternative to the toxic PbTe for high-efficiency mid-temperature thermoelectric applications. However, pristine GeTe suffers from a high concentration of Ge vacancies, resulting in an excessively high hole concentration (> 1 × 1021 cm−3), which greatly limits its thermoelectric enhancement. To address this issue, CuBiTe2 alloying is introduced to increase the formation energy of Ge vacancies in GeTe, thereby inhibiting the high carrier concentration. The carrier scattering caused by the electronegativity difference between different elements is suppressed due to the similar electronegativity of Cu and Ge atoms. A relatively high hole mobility is obtained, which ultimately leads to a high power factor. Additionally, by introducing Se as an alloying element at the anionic site in GeTe, dense point defects with mass/strain-field fluctuations are induced. This contributes to the strengthening of phonon scattering, thereby reducing the lattice thermal conductivity from 1.44 W·m−1·K−1 for pristine GeTe to 0.28 W·m−1·K−1 for Ge0.95Cu0.05Bi0.05Te0.9Se0.15 compound at 623 K.

Graphical abstract

摘要

IV–VI 化合物GeTe被认为是一种很有前途的, 替代有毒PbTe的高效中温热电材料。然而, 本征GeTe存在高浓度的Ge空位, 导致空穴浓度过高（> 1021 cm−3), 极大地限制了其热电性能。为了解决这一问题, 通过CuBiTe2合金化来增加 GeTe 中Ge空位的形成能, 从而抑制高载流子浓度（nH）。同时由于Cu和Ge原子的电负性相似, 抑制了不同元素之间电负性差异引起的载流子散射, 得到高空穴迁移率（μH）, 最终获得了超高功率因子。此外，通过在GeTe的阴离子位置加入Se作为合金化元素, 引入具有质量/应变场波动的致密点缺陷, 极大的加强了声子散射, 在623 K时, 晶格热导率由本征GeTe的1.44 W·m−1K−1降低到Ge0.95Cu0.05Bi0.05Te0.9Se0.15化合物的0.28 W·m−1K−1。最终, Ge0.95Cu0.05Bi0.05Te0.9Se0.15样品在623K时达到最大ZT = ~ 1.87, 在 300–723 K温度范围内, ZTavg显著提高至1.07。本研究成功地优化了GeTe基材料热电传输性能, 为无铅热电材料的探索奠定了坚实的基础。

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Acknowledgements

This work was financially supported by the National Key Research and Development Program of China (No. 2018YFA0702100), National Natural Science Foundation of China (No. U21A2054). K. Guo acknowledges the support from Key Discipline of Materials Science and Engineering, Bureau of Education of Guangzhou (No. 202255464).

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  1. School of Physics and Materials Science, Guangzhou University, Guangzhou, 510006, China

    Xiao-Qiang Wang, Xiao-Quan Hu, Jun-Yan Lin, Chu-Bin Li, Han Li, Shuan-Kui Li & Kai Guo

  2. Research Center for Advanced Information Materials (CAIM), Huangpu Research & Graduate School of Guangzhou University, Sino-Singapore Guangzhou Knowledge City, Guangzhou, 510555, China

    Xiao-Qiang Wang, Xiao-Quan Hu, Han Li, Shuan-Kui Li & Kai Guo

  3. School of Materials Science and Engineering, Shanghai University, Shanghai, 200444, China

    Xiao-Tong Yu & Ji-Ye Zhang

  4. Materials Genome Institute, Shanghai University, Shanghai, 200444, China

    Qi-Yong Chen & Li-Li Xi

  5. School of Mechanical and Mining Engineering, University of Queensland, Brisbane, QLD, 4072, Australia

    Qi-Shuo Yang

  6. Key Laboratory of Si-Based Information Materials & Devices and Integrated Circuits Design, Department of Education of Guangdong Province, Guangzhou, 510006, China

    Kai Guo

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Wang, XQ., Hu, XQ., Lin, JY. et al. Achieving high carrier mobility and low lattice thermal conductivity in GeTe-based alloys by cationic/anionic co-doping. Rare Met. 43, 2784–2795 (2024). https://doi.org/10.1007/s12598-023-02606-4

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  • DOI: https://doi.org/10.1007/s12598-023-02606-4

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