Carrier-phonon decoupling in perovskite thermoelectrics via entropy engineering

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 SrTiO<sub>3</sub>-based perovskite thermoelectrics. By high-entropy design, the lattice thermal conductivity could be reduced nearly to the amorphous limit, 1.25 W m<sup>-1</sup> K<sup>-1</sup>. Simultaneously, entropy engineering can tune the Ti displacement, improving the weighted mobility to 65 cm<sup>2</sup> V<sup>-1</sup> s<sup>-1</sup>. Such carrier-phonon decoupling behaviors enable the greatly enhanced μ<sub>W</sub>/κ<sub>L</sub> of ~5.2 × 10<sup>3</sup> cm<sup>3</sup> K J<sup>-1</sup> V<sup>-1</sup>. The measured maximum zT of 0.24 at 488 K and the estimated zT of ~0.8 at 1173 K in (Sr<sub>0.2</sub>Ba<sub>0.2</sub>Ca<sub>0.2</sub>Pb<sub>0.2</sub>La<sub>0.2</sub>)TiO<sub>3</sub> 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.

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Publication Details

Journal
Nature Communications
Published
2024-09-03
DOI
https://doi.org/10.1038/s41467-024-52063-5
Citations
40
Primary Topic
Advanced Thermoelectric Materials and Devices
Type
article
Field-Weighted Citation Impact
4.69

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article

Carrier-phonon decoupling in perovskite thermoelectrics via entropy engineering

Yueyang Yang, Lvye Dou, Yang Lu, Lin Gu et al.
40 citations
Nature Communications
Advanced Thermoelectric Materials and Devices
4.69
article

Carrier-phonon decoupling in perovskite thermoelectrics via entropy engineering

Yueyang Yang, Lvye Dou, Yang Lu, Lin Gu, Bin Wei, Weigang Ma, Di Yi, Yunpeng Ma, Changpeng Lin, Yunpeng Zheng, Hetian Chen, Jinle Lan, Mingchu Zou, Ce‐Wen Nan, Chang Liu, Dongliang Yang, Zhifang Zhou, Wei Xu, Qinghua Zhang, Qian Li, Wenyu Zhang, Xing Zhang, Yujun Zhang, Jian Han, Yuanhua Lin, Caijuan Shi, Bingbing Yang
article en
40 citations

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 SrTiO<sub>3</sub>-based perovskite thermoelectrics. By high-entropy design, the lattice thermal conductivity could be reduced nearly to the amorphous limit, 1.25 W m<sup>-1</sup> K<sup>-1</sup>. Simultaneously, entropy engineering can tune the Ti displacement, improving the weighted mobility to 65 cm<sup>2</sup> V<sup>-1</sup> s<sup>-1</sup>. Such carrier-phonon decoupling behaviors enable the greatly enhanced μ<sub>W</sub>/κ<sub>L</sub> of ~5.2 × 10<sup>3</sup> cm<sup>3</sup> K J<sup>-1</sup> V<sup>-1</sup>. The measured maximum zT of 0.24 at 488 K and the estimated zT of ~0.8 at 1173 K in (Sr<sub>0.2</sub>Ba<sub>0.2</sub>Ca<sub>0.2</sub>Pb<sub>0.2</sub>La<sub>0.2</sub>)TiO<sub>3</sub> 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.

Nature CommunicationsVol. 15(1)
Chinese Academy of Sciences (CN), Rome International Center for Materials Science (IT), Institute of High Energy Physics (CN), Institute of Solid State Physics (CN), Institute of Physics (CN), National Laboratory for Superconductivity (CN), Henan Polytechnic University (CN), State Key Laboratory of New Ceramics and Fine Processing, École Polytechnique Fédérale de Lausanne (CH), Beijing University of Chemical Technology (CN), Fuzhou University (CN), Tsinghua University (CN)
National Science Foundation, National Natural Science Foundation of China, China Postdoctoral Science Foundation, Tsinghua University
Affordable and clean energy
Openalex Percentile: Top 2%
Advanced Thermoelectric Materials and Devices
4.69
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