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Enhanced thermoelectric performance enabled by compositing ZrO2 in n-type SiGe alloy with low thermal conductivity

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Abstract

SiGe-based thermoelectric (TE) materials have gained increasing interests due to their low maintenance costs, environmental friendliness and long lifespan. However, the intrinsically high thermal conductivity of Si-based materials also results in poor TE properties. In this investigation, a zirconia (ZrO2) composite strategy was applied to an n-type SiGe alloy, tremendously elevating its TE performance. After mechanical alloying and spark plasma sintering (SPS) processes, the ZrO2 induced the formation of nanopores in the SiGe matrix via phosphorus adsorption. Moreover, such increase in porosity enhanced the phonon scattering and dramatically suppressed lattice thermal conductivity, from 2.83 to 1.59 W·m−1·K−1 at 873 K. Additionally, reduced phosphorus doping led to an increase in Seebeck coefficients and a relatively minor decrease in electrical conductivity. The power factor didn’t deteriorate significantly, either, as its maximum of ~ 3.43 mW·m−1·K−2 was achieved at 873 K with (Si0.8Ge0.2)0.097P0.03(ZrO2)0.003. In short, a peak figure of merit (ZT) of ~ 1.27 at 873 K and an average ZT ~ 0.7 from 323 to 873 K were obtained. This study demonstrates that the electrical and thermal transportation of SiGe material can be synergistically tuned by compositing ZrO2, illustrating a novel strategy to optimize the TE properties of bulk materials.

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摘要

硅锗基热电 (TE) 材料因其低维护成本, 环保性和长寿命而受到越来越多的关注. 然而, 硅锗基材料固有的高热导率也导致了其糟糕的TE性能. 在本研究中, 一种氧化锆 (ZrO2) 复合策略被应用于n型硅锗合金中, 极大地提升了其TE性能. 经过机械合金化和火花等离子烧结 (SPS) 过程后, ZrO2 通过磷吸附诱导了硅锗基体中纳米孔的形成. 此外, 这种孔隙率的出现增强了声子散射, 极大地抑制了晶格热导率, 从873 K的 2.83 W m−1·K−1 降至 1.59 W·m−1·K−1. 此外, 磷掺杂的减少导致s赛贝克系数的增加和电导率的小幅下降. 功率因子没有显著恶化, 873 K时(Si0.8Ge0.2)0.97P0.03(ZrO2)0.003其最大功率因子为 3.43 mW·m−1·K−2. 总之, 我们制备的氧化锆复合硅锗热电材料在873 K的峰值ZT为 1.27， 从 323 到 873 K的平均ZT为 0.7. 本研究表明, 通过复合 ZrO2, 硅锗材料的电s输运和热传导可以协同调控, 这展示了一种优化块材料r热电性能的新颖策略.

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Acknowledgements

This work was financially supported by the National Key Research and Development Program of China (Nos. 2022YFE0119100 and 2017YFE0198000), the National Natural Science Foundation of China (Nos. U21A2054, 52273285, 52061009 and 52262032) and Guangxi Science and Technology Planning Project (No. AD21220056).

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Authors and Affiliations

  1. Guangxi Key Laboratory for Relativity Astrophysics, State Key Laboratory of Featured Metal Materials and Life-Cycle Safety for Composite Structures, School of Physical Science and Technology, Guangxi University, Nanning, 530004, China

    Meng-Fei Wang, Ji-Sheng Liang, Wang-Yang Ding, Qi Zhou & Lei Miao

  2. Guangxi Academy of Sciences, Nanning, 530007, China

    Hua-Jun Lai

  3. Key Laboratory of Information Material, Engineering Research Center of Electronic Information Materials and Devices, Guilin University of Electronic Technology, Ministry of Education, Guilin, 541004, China

    Jun-Liang Chen, Ying Peng & Cheng-Yan Liu

  4. Guangxi Key Laboratory of Precision Navigation Technology and Application, School of Information and Communication, Guilin University of Electronic Technology, Guilin, 541004, China

    Ying Peng

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  1. Meng-Fei Wang
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Wang, MF., Lai, HJ., Liang, JS. et al. Enhanced thermoelectric performance enabled by compositing ZrO2 in n-type SiGe alloy with low thermal conductivity. Rare Met. 43, 1167–1176 (2024). https://doi.org/10.1007/s12598-023-02469-9

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