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

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 (λ<sub>ele</sub> ~ 10<sup>3</sup> nm) is found of two orders of magnitude larger than that of phonons (λ<sub>ph</sub> ~ 10<sup>1 </sup>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 Bi<sub>0.88</sub>Sb<sub>0.12</sub> polycrystal, with a ZT<sub>max</sub> of 0.48 at 150 K, is fabricated and demonstrates a ΔT<sub>max</sub> of 4 K at a T<sub>h</sub> of 75 K. This marks the first report of n-p paired thermoelectric cooling modules operating below liquid nitrogen temperature.

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Publication Details

Journal
Nature Communications
Published
2025-04-14
DOI
https://doi.org/10.1038/s41467-025-58491-1
Citations
9
Primary Topic
Advanced Thermoelectric Materials and Devices
Type
article
Field-Weighted Citation Impact
4.66

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article

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

Xin Qian, Ronggui Yang, Zhen Lu, Jun Li et al.
9 citations
Nature Communications
Advanced Thermoelectric Materials and Devices
4.66
article

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

Xin Qian, Ronggui Yang, Zhen Lu, Jun Li, Huaizhou Zhao, Hangtian Zhu, Te‐Huan Liu, Xiaowei Wu, Xiaoyan Niu, Tianyu Wang, Shufang Wang, Nan Chen, Meng Liu, Guodong Li, Zhiliang Li, Zhen Fan, Qi Zhao, Qiulin Liu
article en
9 citations

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 (λ<sub>ele</sub> ~ 10<sup>3</sup> nm) is found of two orders of magnitude larger than that of phonons (λ<sub>ph</sub> ~ 10<sup>1 </sup>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 Bi<sub>0.88</sub>Sb<sub>0.12</sub> polycrystal, with a ZT<sub>max</sub> of 0.48 at 150 K, is fabricated and demonstrates a ΔT<sub>max</sub> of 4 K at a T<sub>h</sub> of 75 K. This marks the first report of n-p paired thermoelectric cooling modules operating below liquid nitrogen temperature.

Nature CommunicationsVol. 16(1)
Chinese Academy of Sciences (CN), Peking University (CN), FZU ‒ Institute of Physics of the Academy of Sciences of the Czech Republic (CZ), Institute of Physics (CN), National Laboratory for Superconductivity (CN), University of Chinese Academy of Sciences (CN), Hebei University (CN), Huazhong University of Science and Technology (CN)
National Natural Science Foundation of China, Huazhong University of Science and Technology, National Key Research and Development Program of China
Affordable and clean energy
Openalex Percentile: Top 5%
Advanced Thermoelectric Materials and Devices
4.66
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