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<p>Lattice distortion realized by entropy engineering can significantly optimize thermoelectric performance through intensifying phonon scattering. However, excessive lattice distortion in high-entropy materials inevitably hinders carrier transport, thereby limiting the wide-temperature average <i>ZT</i> (<i>ZT</i><sub>ave</sub>) value. To enhance the wide-temperature thermoelectric performance of low-cost PbS-based compounds, this work introduces moderate lattice distortion by controlling the entropy around 1.0<i>R</i> (<i>R</i> is the gas constant) to balance phonon and carrier transport, alleviating restrictions on carrier mobility. Firstly, substantial Se and Te alloying in PbS induces rock-salt lattice distortion, which effectively impedes phonon propagation, thus suppressing the lattice thermal conductivity (<i>κ</i><sub>lat</sub>) from 2.41 W m<sup>−1</sup> K<sup>−1</sup> in PbS to 0.66 W m<sup>−1</sup> K<sup>−1</sup> in PbS<sub>0.5</sub>Se<sub>0.35</sub>Te<sub>0.15</sub> at 300 K. Additionally, Cu interstitials are introduced into the lattice-distorted PbS<sub>0.5</sub>Se<sub>0.35</sub>Te<sub>0.15</sub> to further optimize the carrier density and weighted carrier mobility (<i>μ</i><sub>W</sub>), leading to a significant improvement in <i>μ</i><sub>W</sub>/<i>κ</i><sub>lat</sub> parameter at 300–773 K. Finally, a room-temperature <i>ZT</i> of 0.53 and a maximum <i>ZT</i> of 1.44 are obtained in a PbS<sub>0.5</sub>Se<sub>0.35</sub>Te<sub>0.15</sub>-1%Cu sample, which contributes to an impressive <i>ZT</i><sub>ave</sub> of 1.08 at 300–773 K and a maximum power generation efficiency (<i>η</i><sub>max</sub>) 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.</p>

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Realizing broad-range thermoelectric performance in PbS through distorting rock-salt lattice

  • 期刊论文

  • 发表日期：

    2026年4月28日

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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

摘要

Lattice distortion realized by entropy engineering can significantly optimize thermoelectric performance through intensifying phonon scattering. However, excessive lattice distortion in high-entropy materials inevitably hinders carrier transport, thereby limiting the wide-temperature average ZT (ZTave) value. To enhance the wide-temperature thermoelectric performance of low-cost PbS-based compounds, this work introduces moderate lattice distortion by controlling the entropy around 1.0R (R is the gas constant) to balance phonon and carrier transport, alleviating restrictions on carrier mobility. Firstly, substantial Se and Te alloying in PbS induces rock-salt lattice distortion, which effectively impedes phonon propagation, thus suppressing the 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 the carrier density and weighted carrier mobility (μW), leading to a 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 a PbS0.5Se0.35Te0.15-1%Cu sample, which contributes 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.