Carrier-phonon decoupling in perovskite thermoelectrics via entropy engineering.

Zheng, Yunpeng; Zhang, Qinghua; Shi, Caijuan; Zhou, Zhifang; Lu, Yang; Han, Jian; Chen, Hetian; Ma, Yunpeng et al. · Nat Commun · 2024

basic_science · Level V

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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.