Abstract
Thermoelectric devices require thermoelectric materials with high figure-of-merit (ZT) values in the operating temperature range. In recent years, the Zintl phase compound, n-Mg3Sb2, has received much attention owing to its rich chemistry and structural complexity. However, it hardly achieves high ZT values throughout the medium temperature range. Herein, by increasing the sintering temperature as much as possible, we successfully increased the average grain size of the compound by 15 times, and the grain boundary scattering was manipulated to obtain high carrier mobility of up to 180 cm2 V−1 s−1. Simultaneously, we optimized the Mg content for ultralow lattice thermal conductivity. We first doped the Mg3Sb2-based materials with boron for higher sintering temperature, good thermal stability, and higher hardness. The synergistic optimization of electrical and thermal transport resulted in excellent ZT values (0.62 at 300 K, 1.81 at 773 K) and an average ZT of 1.4 (from 300 to 773 K), which are higher than the state-of-the-art values for n-type thermoelectric materials, demonstrating a high potential in device applications.
摘要
器件应用要求热电材料在服役温度范围内具有持续的高热 电优值. 近年来, Zintl相化合物n-Mg3Sb2由于丰富的化学性质和结 构复杂性而受到广泛关注, 但是, n-Mg3Sb2难以在整个中温范围内 保持良好的热电性能. 本文通过提高烧结温度, 使合金平均晶粒尺 寸增加了15倍, 调控了晶界散射从而使载流子迁移率提高至 180 cm2 V−1 s−1. 同时, 更高的烧结温度优化了Mg成分以获得超低 晶格热导率; 采用硼掺杂获得了良好的热稳定性和更高的硬度. 电 热输运特性的协同优化使得硼掺杂Mg3Sb2合金的热电性能在全温 域提高明显, 热电优值为0.62 (300 K)–1.81 (773 K), 在300–773 K之 间的平均热电优值高达1.4, 在热电器件应用方面极具潜力.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (51771065 and 51871082) and the Natural Science Foundation of Heilongjiang Province of China (ZD2020E003).
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Chen X and Sui J designed the experiment. Chen X and Qu N conducted the sample synthesis and performance testing. Qin D, Xue W and Wang Y performed the microstructure characterization. Chen X, Guo f, and Zhu J wrote this article with support and guidance from Cai W, Zhang Q, and Sui J. All authors contributed to the general discussion.
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Xiaoxi Chen received his PhD degree in 2020 in materials science and engineering from Harbin Institute of Technology, China. His main research interests focus on the fabrication and properties of Zintl phase thermoelectric materials.
Jianbo Zhu is a PhD candidate in materials science and engineering at Harbin Institute of Technology. He received his BE degree from Harbin Institute of Technology in 2019. He mainly studies transport problems of electron and phonon using Boltzmann transport equation and first principles calculations.
Fengkai Guo is now a postdoctoral researcher at Harbin Institute of Technology, China. He received his doctorate in material science from Harbin Institute of Technology, China in 2020. His main research interests focus on the fabrication and properties of thermoelectric materials.
Jiehe Sui is currently a professor of material physics and chemistry at Harbin Institute of Technology. He received his PhD degree in materials science and engineering from Harbin Institute of Technology in 2006. After that, he spent two years as a visiting scholar at the University of Houston (2013–2015). His current research is mainly on thermoelectric materials and devices.
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Excellent thermoelectric performance of boron-doped n-type Mg3Sb2-based materials via the manipulation of grain boundary scattering and control of Mg content
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Chen, X., Zhu, J., Qin, D. et al. Excellent thermoelectric performance of boron-doped n-type Mg3Sb2-based materials via the manipulation of grain boundary scattering and control of Mg content. Sci. China Mater. 64, 1761–1769 (2021). https://doi.org/10.1007/s40843-020-1559-4
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DOI: https://doi.org/10.1007/s40843-020-1559-4