Thermoelectric Performance of the 2D Bi2Si2Te6 Semiconductor

Luo, Yubo; Ma, Zheng; Hao, Shiqiang; Cai, Songting; Luo, Zhong-Zhen; Wolverton, Christopher; Dravid, Vinayak P.; Yang, Junyou; Yan, Qingyu; Kanatzidis, Mercouri G.

doi:10.1021/jacs.1c12507

Title: Thermoelectric Performance of the 2D Bi₂Si₂Te₆ Semiconductor

Journal Article · Fri Jan 14 00:00:00 EST 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.1c12507· OSTI ID:1867602

^[1]; Ma, Zheng ^[1];

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Huazhong Univ. of Science and Technology, Wuhan (China)
Northwestern Univ., Evanston, IL (United States)
Nanyang Technological Univ. (Singapore)

Bi₂Si₂Te₆, a 2D compound, is a direct band gap semiconductor with an optical band gap of 0.25 eV, and is a promising thermoelectric material. Single-phase Bi₂Si₂Te₆ is prepared by a scalable ball-milling and annealing process and the highly densified polycrystalline samples are prepared by spark plasma sintering. Bi₂Si₂Te₆ shows a p-type semiconductor transport behavior and exhibits an intrinsically low lattice thermal conductivity of ~0.48 Wm^-1K^-1 (cross-plane) at 573 K. The first-principles density functional theory calculations indicate that such low lattice thermal conductivity is derived from the interactions between acoustic phonons and low-lying optical phonons, local vibrations of Bi, the low Debye temperature and strong anharmonicity result from the unique 2D crystal structure and metavalent bonding of Bi₂Si₂Te₆. The Bi₂Si₂Te₆ exhibits an optimal figure of merit ZT of ~0.51 at 623 K, which can be further enhanced by the substitution of Bi with Pb. Pb doping leads to a large increase in power factor S₂σ, from ~4.0 μWcm^-1K-² of Bi₂Si₂Te₆ to ~8.0 μWcm^-1K^-2 of Bi_1.98Pb_0.02Si₂Te₆ at 775 K, owing to the increase in carrier concentration. Moreover, Pb doping induces a further reduction in the lattice thermal conductivity to ~0.38 Wm^-1K^-1 (cross-plane) at 623 K in Bi_1.98Pb_0.02Si₂Te₆,. The simultaneous optimization of the power factor and lattice thermal conductivity achieves a peak ZT of ~0.90 at 723 K and a high average ZT of ~0.66 at 400–773 K in Bi_1.98Pb_0.02Si₂Te₆.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: SC0014520; 52002137; 92163211; 51802070; 51632006; ECCS-1542205; 2018-T2-1-010; 1527200022

OSTI ID:: 1867602

Journal Information:: Journal of the American Chemical Society, Vol. 144, Issue 3; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
Bi2Si2Te6
Sb2Si2Te6
thermoelectric
thermal conductivity
Seebeck coefficient

Title: Thermoelectric Performance of the 2D Bi2Si2Te6 Semiconductor

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References (65)

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Title: Thermoelectric Performance of the 2D Bi₂Si₂Te₆ Semiconductor