Bulk Bi-Sb polycrystals underpinned by high electron/phonon mean free path ratio enabling thermoelectric cooling under 77 K

Xiaowei Wu, Zhen Fan, Hangtian Zhu, Tianyu Wang, Meng Liu, Jun Li, Nan Chen, Qiulin Liu, Zhen Lu, Guodong Li, Xin Qian, Te-Huan Liu (), Ronggui Yang, Xiaoyan Niu, Qi Zhao, Zhiliang Li, Shufang Wang and Huaizhou Zhao ()
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Xiaowei Wu: Chinese Academy of Sciences
Zhen Fan: Chinese Academy of Sciences
Hangtian Zhu: Chinese Academy of Sciences
Tianyu Wang: Huazhong University of Science and Technology
Meng Liu: Chinese Academy of Sciences
Jun Li: Chinese Academy of Sciences
Nan Chen: Chinese Academy of Sciences
Qiulin Liu: Chinese Academy of Sciences
Zhen Lu: Chinese Academy of Sciences
Guodong Li: Chinese Academy of Sciences
Xin Qian: Huazhong University of Science and Technology
Te-Huan Liu: Huazhong University of Science and Technology
Ronggui Yang: Peking University
Xiaoyan Niu: Hebei University
Qi Zhao: Hebei University
Zhiliang Li: Hebei University
Shufang Wang: Hebei University
Huaizhou Zhao: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Bi-Sb alloy, as a promising thermoelectric material at cryogenic temperatures, has seen stagnant progress due to challenges in understanding the transport behaviors of energy carriers, and difficulties in synthesizing high-homogeneity, large-grain samples. In this study, an inherent electron-phonon decoupling in Bi-Sb is revealed using the first-principles calculations based on the virtual crystal approximation. The mean free path of the dominant electrons (λele ~ 103 nm) is found of two orders of magnitude larger than that of phonons (λph ~ 101 nm), suggesting that a grain size greater than 10 μm would be favorable for thermoelectric transport. Bulk Bi-Sb polycrystals with highly elemental homogeneity and large grain size (~80 μm) are successfully synthesized through an ultra-fast quenching method combined with annealing, delivering superior thermoelectric performance. A prototype module based on the Bi0.88Sb0.12 polycrystal, with a ZTmax of 0.48 at 150 K, is fabricated and demonstrates a ΔTmax of 4 K at a Th of 75 K. This marks the first report of n-p paired thermoelectric cooling modules operating below liquid nitrogen temperature.

Date: 2025
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DOI: 10.1038/s41467-025-58491-1

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