Key Takeaways & Executive Findings
- •• • Moderate lattice distortion (entropy ~1.0R) in PbS0.5Se0.35Te0.15 reduces lattice thermal conductivity from 2.41 W m−1 K−1 (PbS) to 0.66 W m−1 K−1 at 300 K, a 73% reduction, enabling efficient phonon scattering without severely compromising carrier mobility. • • Cu interstitial doping (1% Cu) in PbS0.5Se0.35Te0.15 optimizes carrier density and weighted carrier mobility, achieving a room-temperature ZT of 0.53 and a peak ZT of 1.44 at elevated temperatures, demonstrating balanced electrical and thermal transport. • • The engineered material attains a wide-temperature average ZT (ZTave) of 1.08 across 300–773 K, translating to a maximum power generation efficiency (ηmax) of 7.5%, outperforming prior cost-effective PbS-based thermoelectrics. • • The strategy of controlled lattice distortion (entropy ~1.0R) provides a design route for low-cost, earth-abundant thermoelectric materials, achieving performance metrics comparable to high-entropy systems but with less carrier mobility degradation, which is critical for practical waste-heat recovery applications.
Abstract
Lattice distortion via entropy engineering can significantly optimize thermoelectric performance by intensifying phonon scattering. However, excessive lattice distortion in high-entropy materials inevitably hinders carrier transport, limiting the wide-temperature average ZT (ZTave). To enhance the wide-temperature thermoelectric performance of low-cost PbS-based compounds, this work introduces moderate lattice distortion by controlling entropy around 1.0R (R is the gas constant) to balance phonon and carrier transport, alleviating restrictions on carrier mobility. Substantial Se and Te alloying in PbS induces rock-salt lattice distortion, effectively impeding phonon propagation, thus suppressing lattice thermal conductivity (κlat) from 2.41 W m−1 K−1 in PbS to 0.66 W m−1 K−1 in PbS0.5Se0.35Te0.15 at 300 K. Additionally, Cu interstitials are introduced into the lattice-distorted PbS0.5Se0.35Te0.15 to further optimize carrier density and weighted carrier mobility (μW), leading to significant improvement in μW/κlat parameter at 300–773 K. Finally, a room-temperature ZT of 0.53 and a maximum ZT of 1.44 are obtained in PbS0.5Se0.35Te0.15-1%Cu sample, contributing to an impressive ZTave of 1.08 at 300–773 K and a maximum power generation efficiency (ηmax) of 7.5%. The results outperform previously reported cost-effective PbS-based compounds and highlight the importance of lattice distortion regulation in enhancing wide-temperature thermoelectric performance.
1. Introduction
Thermoelectric materials enable direct conversion between heat and electricity, offering a promising route for waste heat recovery. The thermoelectric figure of merit, ZT = S2σT/κ, governs conversion efficiency, but optimizing ZTave across a wide temperature range is challenging due to strong coupling between electrical and thermal transport. High-entropy materials (ΔS > 1.5R) achieve ultralow lattice thermal conductivity via severe lattice distortion, yet this often degrades carrier mobility, limiting ZTave. For instance, high-entropy PbSe-based compounds reach peak ZT ~2.0 at 900 K, but their wide-temperature performance suffers from reduced carrier transport.
This work addresses the bottleneck by introducing moderate lattice distortion (entropy ~1.0R) in PbS, a low-cost, earth-abundant material. By alloying Se and Te, the rock-salt lattice is distorted to suppress phonon propagation while preserving carrier mobility. Cu interstitials further optimize carrier density and weighted mobility. The resulting PbS0.5Se0.35Te0.15-1%Cu achieves a ZTave of 1.08 (300–773 K) and a maximum efficiency of 7.5%, outperforming prior PbS-based systems. This approach demonstrates that controlled lattice distortion, rather than extreme entropy, can balance phonon and carrier transport, offering a practical pathway for high-performance, cost-effective thermoelectrics.
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Wei Liu, Tao Hong, Yu Tian, Liqing Xu, Zhanxiang Yin, Peng Ai, Xinxiu Cheng, Lizhong Su, Haiyuan Chen, Yu Xiao, Li-Dong Zhao (2026). Realizing Broad-Range Thermoelectric Performance in PbS through Distorting Rock-Salt Lattice. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-4017-y
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Frequently Asked Questions
What is the trade-off between lattice distortion and carrier mobility in high-entropy thermoelectrics, and how does this work mitigate it?
High-entropy materials (ΔS > 1.5R) exhibit severe lattice distortion that strongly scatters phonons, reducing lattice thermal conductivity to ~0.3 W m−1 K−1, but also disrupts carrier transport, lowering mobility. This work uses moderate distortion (entropy ~1.0R) in PbS0.5Se0.35Te0.15, achieving a 73% reduction in κlat (from 2.41 to 0.66 W m−1 K−1 at 300 K) while maintaining a weighted carrier mobility sufficient to yield a ZTave of 1.08 (300–773 K). The balance is critical for wide-temperature performance.
How does Cu interstitial doping affect the thermoelectric performance of PbS0.5Se0.35Te0.15?
Cu interstitials (1% Cu) optimize carrier density and weighted carrier mobility (μW), enhancing the μW/κlat ratio across 300–773 K. This leads to a room-temperature ZT of 0.53 and a peak ZT of 1.44, contributing to a ZTave of 1.08 and a maximum efficiency of 7.5%.
What are the practical efficiency and temperature range of the developed material for power generation?
The PbS0.5Se0.35Te0.15-1%Cu sample achieves a maximum power generation efficiency (ηmax) of 7.5% over a temperature gradient from 300 K to 773 K. This wide-temperature capability is essential for waste heat recovery applications where temperature varies.
How does the performance of this material compare to other cost-effective PbS-based thermoelectrics?
The ZTave of 1.08 (300–773 K) and ηmax of 7.5% outperform previously reported cost-effective PbS-based compounds, which typically have ZTave below 0.8. The moderate lattice distortion strategy provides a competitive alternative to high-entropy systems with less carrier mobility degradation.
What is the industrial significance of achieving high ZTave in low-cost PbS?
PbS is abundant and inexpensive compared to Te-based thermoelectrics. Achieving a ZTave of 1.08 over 300–773 K makes PbS viable for mid-temperature waste heat recovery, potentially reducing system costs and enabling broader deployment in industrial and automotive applications.
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