Valence Disproportionation of GeS in the PbS Matrix Forms Pb5Ge5S12 Inclusions with Conduction Band Alignment Leading to High n-Type Thermoelectric Performance

Luo, Zhong-Zhen; Cai, Songting; Hao, Shiqiang; Bailey, Trevor P.; Xie, Hongyao; Slade, Tyler J.; Liu, Yukun; Luo, Yubo; Chen, Zixuan; Xu, Jianwei; Luo, Wenjun; Yu, Yan; Uher, Ctirad; Wolverton, Christopher; Dravid, Vinayak P.; Zou, Zhigang; Yan, Qingyu; Kanatzidis, Mercouri G.

doi:10.1021/jacs.2c01706

Title: Valence Disproportionation of GeS in the PbS Matrix Forms Pb₅Ge₅S₁₂ Inclusions with Conduction Band Alignment Leading to High n-Type Thermoelectric Performance

Journal Article · Thu Apr 14 00:00:00 EDT 2022 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c01706· OSTI ID:1867609

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Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, Fujian (China); Fuzhou Univ. (China); Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States); Huazhong Univ. of Science and Technology, Wuhan (China)
Fuzhou Univ. (China)
Agency for Science, Technology and Research (A*STAR) (Singapore). Institute of Materials Research and Engineering
Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, Fujian (China); Nanjing Univ. (China)
Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, Fujian (China); Fuzhou Univ. (China)
Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, Fujian (China); Fuzhou Univ. (China); Nanjing Univ. (China)
Nanyang Technological Univ. (Singapore)

Converting waste heat into useful electricity using solid-state thermoelectrics has a potential for enormous global energy savings. Lead chalcogenides are among the most prominent thermoelectric materials, whose performance decreases with an increase in chalcogen amounts (e.g., PbTe>PbSe>PbS). Herein, we demonstrate the simultaneous optimization of the electrical and thermal transport properties of PbS-based compounds by alloying with GeS. The addition of GeS triggers a complex cascade of beneficial events as follows: Ge²⁺ substitution in Pb²⁺ and discordant off-center behavior; formation of Pb₅Ge₅S₁₂ as stable second phase inclusions through valence disproportionation of Ge²⁺ to Ge0 and Ge⁴⁺. PbS and Pb₅Ge₅S₁₂ exhibit good conduction band energy alignment that preserves the high electron mobility; the formation of Pb₅Ge₅S₁₂ increases the electron carrier concentration by introducing S vacancies. Sb doping as the electron donor produces a large power factor and low lattice thermal conductivity (κ_lat) of ~0.61 Wm^-1K^-1. The highest performance was obtained for the 14% GeS-alloyed samples, which exhibited an increased room temperature electron mobility of ~121 cm²V^-1s^-1 for 3 × 10¹⁹ cm^-3 carrier density, and a ZT, of 1.32 at 923 K. This is ~ 55% greater that the corresponding Sb-doped PbS sample and is one of the highest reported for the n-type PbS system. Moreover, the average ZT (ZT_avg) of ~0.76 from 400 to 923 K is the highest for PbS-based systems.

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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; A19D9a0096; 2020YFA0710303; 2018-T2-1-010; ECCS-1542205; 52102218; 61728401; DMR-1720139; 2021ZZ127

OSTI ID:: 1867609

Journal Information:: Journal of the American Chemical Society, Vol. 144, Issue 16; 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
54 ENVIRONMENTAL SCIENCES
42 ENGINEERING
Waste heat harvesting
n-type PbS
Pb5Ge5S12
conduction band alignment
all-scale hierarchical architectures

Title: Valence Disproportionation of GeS in the PbS Matrix Forms Pb5Ge5S12 Inclusions with Conduction Band Alignment Leading to High n-Type Thermoelectric Performance

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Title: Valence Disproportionation of GeS in the PbS Matrix Forms Pb₅Ge₅S₁₂ Inclusions with Conduction Band Alignment Leading to High n-Type Thermoelectric Performance