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Here, we investigate PbSnS2, a wide band gap (1.13 eV) compound, as a promising thermoelectric material for power generation. Single crystal X-ray diffraction analysis reveals its 2D-layered structure, akin to the GeSe structure type, with Pb and Sn atoms sharing the same crystallographic site. The polycrystalline PbSnS2 exhibits an intrinsically ultralow lattice thermal conductivity (kappa(lat)) of 0.37 W m(-1) K-1 at 573 K. However, the low carrier concentration (n) leads to suboptimal electrical conductivity (sigma), capping the ZT value at 0.1. Accordingly, the halogen elements (Cl, Br, and I) are employed as the n-type dopants to improve the n. The DFT results indicate a significant weakening of Pb/Sn & horbar;S bonds upon halogen-doping, contributing to the observed reduction in kappa(lat). Our analysis indicates the activation of multiconduction band transport driven by halogen substitution. The PbSnS1.96Br0.04 has a high power factor of five times that of intrinsic PbSnS2. Halogen-doping weakens the Pb/Sn & horbar;S bonds and enhances the phonon scattering, leading to an ultralow kappa(lat) of 0.29 W m(-1) K-1 at 873 K for PbSnS1.96Br0.04. Consequently, PbSnS1.96Br0.04 achieved a maximum ZT value of 0.82 at 873 K.
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Year: 2025
Issue: 21
Volume: 64
1 6 . 1 0 0
JCR@2023
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