High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe3 by High-Entropy Engineering

Luo, Yubo; Hao, Shiqiang; Cai, Songting; Slade, Tyler J.; Luo, Zhong Zhen; Dravid, Vinayak P.; Wolverton, Chris; Yan, Qingyu; Kanatzidis, Mercouri G.

doi:10.1021/jacs.0c07803

Title: High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe₃ by High-Entropy Engineering

Journal Article · Tue Aug 04 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c07803· OSTI ID:1778875

^[1]; Hao, Shiqiang ^[2];

^[2];

^[2]; Luo, Zhong Zhen ^[3];

^[2];

^[4];

^[2]

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

We investigate the structural and physical properties of the AgSn_mSbSe_m+2 system with m = 1-20 (i.e., SnSe matrix and ~5-50% AgSbSe₂) from atomic, nano, and macro length scales. We find the 50:50 composition, with m = 1 (i.e., AgSnSbSe₃), forms a stable cation-disordered cubic rock-salt p-type semiconductor with a special multi-peak electronic valence band structure. AgSnSbSe₃ has an intrinsically low lattice thermal conductivity of ~0.47 W m^-1 K^-1 at 673 K owing to the synergy of cation disorder, phonon anharmonicity, low phonon velocity, and low-frequency optical modes. Furthermore, Te alloying on Se sites creates a quinary high-entropy NaCl-type solid solution AgSnSbSe_3-xTe_x with randomly disordered cations and anions. The extra point defects and lattice dislocations lead to glass-like lattice thermal conductivities of ~0.32 W m^-1 K^-1 at 723 K and higher hole carrier concentration than AgSnSbSe₃. Concurrently, the Te alloying promotes greater convergence of the multiple valence band maxima in AgSnSbSe_1.5Te_1.5, the composition with the highest configurational entropy. Facilitated by these favorable modifications, we achieve a high average power factor of ~9.54 μW cm^-1 K^-2 (400-773 K), a peak thermoelectric figure of merit ZT of 1.14 at 723 K, and a high average ZT of ~1.0 over a wide temperature range of 400-773 K in AgSnSbSe_1.5Te_1.5.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0014520

OSTI ID:: 1778875

Journal Information:: Journal of the American Chemical Society, Vol. 142, Issue 35; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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