Carrier-phonon decoupling in perovskite thermoelectrics via entropy engineering

Yunpeng Zheng, Qinghua Zhang, Caijuan Shi, Zhifang Zhou, Yang Lu, Jian Han, Hetian Chen, Yunpeng Ma, Yujun Zhang, Changpeng Lin, Wei Xu, Weigang Ma, Qian Li, Yueyang Yang, Bin Wei, Bingbing Yang, Mingchu Zou, Wenyu Zhang, Chang Liu, Lvye Dou, Dongliang Yang, Jin-Le Lan, Di Yi, Xing Zhang, Lin Gu, Ce-Wen Nan and Yuan-Hua Lin ()
Additional contact information
Yunpeng Zheng: Tsinghua University
Qinghua Zhang: Chinese Academy of Sciences
Caijuan Shi: Chinese Academy of Sciences
Zhifang Zhou: Tsinghua University
Yang Lu: Tsinghua University
Jian Han: Tsinghua University
Hetian Chen: Tsinghua University
Yunpeng Ma: Tsinghua University
Yujun Zhang: Chinese Academy of Sciences
Changpeng Lin: École Polytechnique Fédérale de Lausanne
Wei Xu: Chinese Academy of Sciences
Weigang Ma: Tsinghua University
Qian Li: Tsinghua University
Yueyang Yang: Tsinghua University
Bin Wei: Tsinghua University
Bingbing Yang: Tsinghua University
Mingchu Zou: Tsinghua University
Wenyu Zhang: Tsinghua University
Chang Liu: Tsinghua University
Lvye Dou: Tsinghua University
Dongliang Yang: Chinese Academy of Sciences
Jin-Le Lan: Beijing University of Chemical Technology
Di Yi: Tsinghua University
Xing Zhang: Tsinghua University
Lin Gu: Tsinghua University
Ce-Wen Nan: Tsinghua University
Yuan-Hua Lin: Tsinghua University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Thermoelectrics converting heat and electricity directly attract broad attentions. To enhance the thermoelectric figure of merit, zT, one of the key points is to decouple the carrier-phonon transport. Here, we propose an entropy engineering strategy to realize the carrier-phonon decoupling in the typical SrTiO3-based perovskite thermoelectrics. By high-entropy design, the lattice thermal conductivity could be reduced nearly to the amorphous limit, 1.25 W m−1 K−1. Simultaneously, entropy engineering can tune the Ti displacement, improving the weighted mobility to 65 cm2 V−1 s−1. Such carrier-phonon decoupling behaviors enable the greatly enhanced μW/κL of ~5.2 × 103 cm3 K J−1 V−1. The measured maximum zT of 0.24 at 488 K and the estimated zT of ~0.8 at 1173 K in (Sr0.2Ba0.2Ca0.2Pb0.2La0.2)TiO3 film are among the best of n-type thermoelectric oxides. These results reveal that the entropy engineering may be a promising strategy to decouple the carrier-phonon transport and achieve higher zT in thermoelectrics.

Date: 2024
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DOI: 10.1038/s41467-024-52063-5

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