Microstructural transformation for robust and high-efficiency Zintl thermoelectrics

Meng Jiang, Qinghua Zhang, Siyuan Zhang (), Ming Liu, Yuntian Fu, Zhiyuan Zhang, Xin Ai (), Bohayra Mortazavi, Lianjun Wang (), Qihao Zhang (), Denys Makarov and Wan Jiang
Additional contact information
Meng Jiang: Donghua University
Qinghua Zhang: Welfengarten 1A
Siyuan Zhang: Max-Planck-Straße 1
Ming Liu: RWTH Aachen University
Yuntian Fu: Donghua University
Zhiyuan Zhang: Max-Planck-Straße 1
Xin Ai: Leibniz Institute for Solid State and Materials Research Dresden e.V
Bohayra Mortazavi: Welfengarten 1A
Lianjun Wang: Donghua University
Qihao Zhang: Donghua University
Denys Makarov: Institute of Ion Beam Physics and Materials Research
Wan Jiang: Donghua University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Thermoelectric materials offer an exceptional opportunity to convert waste heat into electricity directly, yet their widespread application remains hindered by intrinsic brittleness and poor processability. Here, we introduce a graded ball milling strategy that fundamentally enhances the mechanical robustness and processability of YbZn2Sb2-based thermoelectrics. By refining grain microstructure, increasing dislocation density, and promoting intermediate-angle grain boundaries, this approach enables the fabrication of crack-free, large-size, disc-shaped, and microscale dices while maintaining excellent thermoelectric performance. Extending this strategy to a broader class of brittle Zintl compounds, including AZn2Sb2, AMg2Sb2, and ACd2Sb2 (A = Yb, Mg, Ca, Sr, Ba), we achieve a pre-formation cohesive energy of 9.1 eV atom−1 and relatively low lattice thermal conductivity of 0.5 W m−1 K−1 in Yb0.5Mg1.3Zn1.2Sb2. Integrated with n-type Mg3.1Nb0.1Sb1.5Bi0.49Te0.01, the thermoelectric module achieves a conversion efficiency exceeding 10% under a 458 K temperature gradient, operating for more than 40 hours steadily. This work establishes a scalable and versatile strategy for reconciling mechanical durability with high thermoelectric performance, paving the way for next-generation thermoelectric devices with enhanced reliability and industrial viability.

Date: 2025
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DOI: 10.1038/s41467-025-62660-7

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