Ultralow Thermal Conductivity and High-Temperature Thermoelectric Performance in n-Type K2.5Bi8.5Se14

Luo, Zhong-Zhen; Cai, Songting; Hao, Shiqiang; Bailey, Trevor P.; Hu, Xiaobing; Hanus, Riley; Ma, Runchu; Tan, Gangjian; Chica, Daniel G.; Snyder, G. Jeffrey; Uher, Ctirad; Wolverton, Christopher; Dravid, Vinayak P.; Yan, Qingyu; Kanatzidis, Mercouri G.

doi:10.1021/acs.chemmater.9b02327

Title: Ultralow Thermal Conductivity and High-Temperature Thermoelectric Performance in n-Type K_2.5Bi_8.5Se₁₄

Journal Article · Thu Jul 11 00:00:00 EDT 2019 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b02327· OSTI ID:1776869

^[1]; Cai, Songting ^[2];

^[2]; Bailey, Trevor P. ^[3];

^[2]; Hanus, Riley ^[2]; Ma, Runchu ^[3]; Tan, Gangjian ^[4]; Chica, Daniel G. ^[2]; Snyder, G. Jeffrey ^[2]; Uher, Ctirad ^[3];

^[2];

^[5];

^[2]

Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Wuhan Univ. of Technology, Wuhan (China)
Nanyang Technological Univ. (Singapore)

We studied the narrow band-gap (0.55 eV) semiconductor K_2.5Bi_8.5Se₁₄ as a potential thermoelectric material for power generation. Samples of polycrystalline K_2.5Bi_8.5Se₁₄ prepared by spark plasma sintering exhibit exceptionally low lattice thermal conductivities (κ_lat) of 0.57-0.33 W m^-1 K^-1 in the temperature range of 300-873 K. The physical origin of such low κ_lat in K_2.5Bi_8.5Se₁₄ is related to the strong anharmonicity and low phonon velocity caused by its complex low symmetry, large unit cell crystal structure, and mixed occupancy of Bi and K atoms in the lattice. High-resolution scanning transmission electron microscopy studies and microanalysis indicate that the K_2.5Bi_8.5Se₁₄ sample is a single phase without intergrowth of the structurally related K₂Bi₈Se₁₃ phase. The undoped material exhibits an n-type character and a figure-of-merit (ZT) value of 0.67 at 873 K. Electronic band structure calculations indicate that K_2.5Bi_8.5Se₁₄ is an indirect band-gap semiconductor with multiple conduction bands close to the Fermi level. Phonon dispersion calculations suggest that K_2.5Bi_8.5Se₁₄ has low phonon velocities and large Grüneisen parameters that can account for the observed ultralow κ_lat. The degree of n-type doping can be controlled by introducing Se deficiencies in the structure, providing a simple route to increase the ZT to ~1 at 873 K.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); International Institute for Nanotechnology (IIN); Keck Foundation

Grant/Contract Number:: SC0014520; AC02-06CH11357; AC02-05CH11231; 2018-T2-1-01; MOE2017-T2-2-0690

OSTI ID:: 1776869

Journal Information:: Chemistry of Materials, Vol. 31, Issue 15; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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Title: Ultralow Thermal Conductivity and High-Temperature Thermoelectric Performance in n-Type K_2.5Bi_8.5Se₁₄