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<p>Rock-salt-structured compounds like lead chalcogenides are promising thermoelectrics, as their high symmetry, strong anharmonicity, and favorable phase behavior collectively lead to high performance by enabling large power factors and ultralow thermal conductivity. Here, we report LiMnSbTe<sub>3</sub>, a new rock-salt semiconductor stabilized through targeted chemical design by combining hexagonal MnTe with cubic LiSbTe<sub>2</sub>. Embedded in the high-symmetry matrix, van der Waals-like gaps form due to Sb<sub>2</sub>Te<sub>3</sub> nanoscale segregation, which acts as effective phonon-scattering centers, leading to a low lattice thermal conductivity of 0.37 Wm<sup>-1</sup>K<sup>-1</sup> at 873 K with alloy scattering from disordered cations. The ordered local structure of Sb<sub>2</sub>Te<sub>3</sub>-type vdW-like gaps and the cross-gap interaction facilitate the carrier transport. Aided by energy-converged valence bands and a paramagnon drag effect, high Seebeck coefficients and enhanced power factor can be achieved, leading to a high <i>ZT</i> of 1.2 at 873 K. Furthermore, introducing Mn deficiency increases <i>ZT</i> to 1.5, highlighting the potential for higher performance through optimized doping or alloying. A segmented single-leg thermoelectric module achieves an output power density of 0.52 Wcm<sup>-2</sup> and an efficiency of 8.7% under ∆<i>T</i> of 478 K, further demonstrating its promising thermoelectric applications.</p>

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Stabilization of high-performance rock-salt LiMnSbTe3 thermoelectrics with embedded van der Waals-like gaps

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月20日

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  • Jinfeng Dong,
  • Yukun Liu,
  • Yandong Sun,
  • Yuan Yu,
  • Yilin Jiang,
  • Chenguang Zhang,
  • Sumayya,
  • Chen Chen,
  • Xian Yi Tan,
  • Li Ping Tan,
  • Paribesh Acharyya,
  • D. V. Maheswar Repaka,
  • Dongwang Yang,
  • Ben Xu,
  • Kedar Hippalgaonkar,
  • R. V. Ramanujan,
  • Jing-Feng Li,
  • Vinayak P. Dravid,
  • Qingyu Yan,
  • Mercouri G. Kanatzidis

摘要

Rock-salt-structured compounds like lead chalcogenides are promising thermoelectrics, as their high symmetry, strong anharmonicity, and favorable phase behavior collectively lead to high performance by enabling large power factors and ultralow thermal conductivity. Here, we report LiMnSbTe3, a new rock-salt semiconductor stabilized through targeted chemical design by combining hexagonal MnTe with cubic LiSbTe2. Embedded in the high-symmetry matrix, van der Waals-like gaps form due to Sb2Te3 nanoscale segregation, which acts as effective phonon-scattering centers, leading to a low lattice thermal conductivity of 0.37 Wm-1K-1 at 873 K with alloy scattering from disordered cations. The ordered local structure of Sb2Te3-type vdW-like gaps and the cross-gap interaction facilitate the carrier transport. Aided by energy-converged valence bands and a paramagnon drag effect, high Seebeck coefficients and enhanced power factor can be achieved, leading to a high ZT of 1.2 at 873 K. Furthermore, introducing Mn deficiency increases ZT to 1.5, highlighting the potential for higher performance through optimized doping or alloying. A segmented single-leg thermoelectric module achieves an output power density of 0.52 Wcm-2 and an efficiency of 8.7% under ∆T of 478 K, further demonstrating its promising thermoelectric applications.