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author:

Chen, Zixuan (Chen, Zixuan.) [1] | Ming, Hongwei (Ming, Hongwei.) [2] | Li, Zhi (Li, Zhi.) [3] | Girard, Steven N. (Girard, Steven N..) [4] | Morris, Collin D. (Morris, Collin D..) [5] | Guo, Weiping (Guo, Weiping.) [6] | Wu, Ming (Wu, Ming.) [7] | Yu, Yan (Yu, Yan.) [8] (Scholars:于岩) | Wolverton, Christopher (Wolverton, Christopher.) [9] | Luo, Zhong-Zhen (Luo, Zhong-Zhen.) [10] (Scholars:罗中箴) | Zou, Zhigang (Zou, Zhigang.) [11] | Kanatzidis, Mercouri G. (Kanatzidis, Mercouri G..) [12]

Indexed by:

EI Scopus SCIE

Abstract:

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.

Keyword:

Halogen-doping PbSnS2 Single crystal Thermoelectricity Ultralow thermal conductivity

Community:

  • [ 1 ] [Chen, Zixuan]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Adv Mat Technol, Int Hong Kong Macao & Taiwan Joint Lab Adv Mat Tec, Fuzhou 350108, Fujian, Peoples R China
  • [ 2 ] [Guo, Weiping]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Adv Mat Technol, Int Hong Kong Macao & Taiwan Joint Lab Adv Mat Tec, Fuzhou 350108, Fujian, Peoples R China
  • [ 3 ] [Wu, Ming]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Adv Mat Technol, Int Hong Kong Macao & Taiwan Joint Lab Adv Mat Tec, Fuzhou 350108, Fujian, Peoples R China
  • [ 4 ] [Yu, Yan]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Adv Mat Technol, Int Hong Kong Macao & Taiwan Joint Lab Adv Mat Tec, Fuzhou 350108, Fujian, Peoples R China
  • [ 5 ] [Luo, Zhong-Zhen]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Adv Mat Technol, Int Hong Kong Macao & Taiwan Joint Lab Adv Mat Tec, Fuzhou 350108, Fujian, Peoples R China
  • [ 6 ] [Zou, Zhigang]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Adv Mat Technol, Int Hong Kong Macao & Taiwan Joint Lab Adv Mat Tec, Fuzhou 350108, Fujian, Peoples R China
  • [ 7 ] [Ming, Hongwei]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China
  • [ 8 ] [Yu, Yan]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China
  • [ 9 ] [Luo, Zhong-Zhen]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China
  • [ 10 ] [Zou, Zhigang]Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Fujian, Peoples R China
  • [ 11 ] [Li, Zhi]Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
  • [ 12 ] [Wolverton, Christopher]Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
  • [ 13 ] [Girard, Steven N.]Univ Wisconsin Whitewater, Dept Chem, 800 W Main St, Whitewater, WI 53190 USA
  • [ 14 ] [Morris, Collin D.]Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
  • [ 15 ] [Kanatzidis, Mercouri G.]Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
  • [ 16 ] [Luo, Zhong-Zhen]Fuzhou Univ, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 17 ] [Zou, Zhigang]Nanjing Univ, Coll Engn & Appl Sci, Ecomat & Renewable Energy Res Ctr, Nanjing 210093, Peoples R China
  • [ 18 ] [Zou, Zhigang]Nanjing Univ, Natl Lab Solid State Microstruct, Nanjing 210093, Peoples R China

Reprint 's Address:

  • 罗中箴

    [Luo, Zhong-Zhen]Fuzhou Univ, Coll Mat Sci & Engn, Key Lab Adv Mat Technol, Int Hong Kong Macao & Taiwan Joint Lab Adv Mat Tec, Fuzhou 350108, Fujian, Peoples R China;;[Kanatzidis, Mercouri G.]Northwestern Univ, Dept Chem, Evanston, IL 60208 USA

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

Year: 2025

Issue: 21

Volume: 64

1 6 . 1 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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