Thermoelectric Material SnPb2Bi2S6: The 4,4L Member of Lillianite Homologous Series with Low Lattice Thermal Conductivity

Li, Jingpeng; Zhou, Yiming; Hao, Shiqiang; Zhang, Tianyan; Wolverton, Chris; Zhao, Jing; Zhao, Li-Dong

doi:10.1021/acs.inorgchem.8b02899

Thermoelectric Material SnPb₂Bi₂S₆: The ^4,4L Member of Lillianite Homologous Series with Low Lattice Thermal Conductivity

Journal Article · Mon Dec 31 04:00:00 EST 2018 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.8b02899· OSTI ID:1776867

^[1]; Zhou, Yiming ^[2]; Hao, Shiqiang ^[3]; Zhang, Tianyan ^[4]; ^[3]; ^[4]; ^[2]

Univ. of Science and Technology, Beijing (China); Northwestern University
Beihang Univ., Beijing (China)
Northwestern Univ., Evanston, IL (United States)
Univ. of Science and Technology, Beijing (China)

Although the binary sulfides Bi₂S₃, PbS, and SnS have attracted extensive interest as thermoelectric materials, no quaternary sulfides containing Sn/Pb/Bi/S elements have been reported. In this paper, we report the synthesis of a new quaternary sulfide, SnPb₂Bi₂S₆, which crystallizes in the orthorhombic space group Pnma with unit cell parameters of a = 20.5458(12) Å, b = 4.0925(4) Å, c = 13.3219(10) Å. SnPb₂Bi₂S₆ has a lillianite-type crystal structure consisting of two alternately aligned NaCl-type structural motifs separated by a mirror plane of PbS₇ monocapped trigonal prisms. In the lillianite homologous series, SnPb₂Bi₂S₆ can be classified as 4,4L, where the superscripted numbers indicate the maximum numbers of edge-sharing octahedra in the two adjacent NaCl-shaped slabs along the diagonal direction. The obtained SnPb₂Bi₂S₆ phase exhibited good thermal stability up to 1000 K and n-type degenerate semiconducting behavior, with a power factor of 3.7 μW cm^-1 K^-2 at 773 K. Notably, this compound exhibited a very low lattice thermal conductivity of 0.69-0.92 W m^-1 K^-1 at 300-1000 K. Theoretical calculations revealed that the low thermal conductivity is caused by the complex crystal structure and the related elastic properties of a low Debye temperature, low phonon velocity, and large Grüneisen parameters. A reasonable figure of merit (ZT) of ~0.3 was obtained at 770 K.

Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Beijing Natural Science Foundation; National Natural Science Foundation of China (NSFC); Fundamental Research Funds for the Central Universities

DOE Contract Number:: SC0014520

OSTI ID:: 1776867

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 2 Vol. 58; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

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