Enhancement of Thermoelectric Performance for n-Type PbS through Synergy of Gap State and Fermi Level Pinning
Abstract
In this paper, we report that Ga-doped and Ga-In-codoped n-type PbS samples show excellent thermoelectric performance in the intermediate temperature range. First-principles electronic structure calculations reveal that Ga doping can cause Fermi level pinning in PbS by introducing a gap state between the conduction and valence bands. Furthermore, Ga-In codoping introduces an extra conduction band. These added electronic features lead to high electron mobilities up to μH ~ 630 cm2 V-1 s-1 for n of 1.67 × 1019 cm-3 and significantly enhanced Seebeck coefficients in PbS. Consequently, we obtained a maximum power factor of ~32 μW cm-1 K-2 at 300 K for Pb0.9875Ga0.0125S, which is the highest reported for PbS-based systems giving a room-temperature figure of merit, ZT, of ~0.35 and ~0.82 at 923 K. For the codoped Pb0.9865Ga0.0125In0.001S, the maximum ZT rises to ~1.0 at 923 K and achieves a record-high average ZT (ZTavg) of ~0.74 in the temperature range of 400-923 K.
- Authors:
-
[1];
[2];
[2];
[2];
[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 (China)
- Nanyang Technological Univ. (Singapore)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Natural Science Foundation of China (NSFC)
- OSTI Identifier:
- 1777108
- Grant/Contract Number:
- SC0014520; AC02- 06CH11357; AC02-05CH11231; 61728401; ECCS-1542205; DMR-1720139
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 15; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thermal conductivity; Band structure; Thermoelectric materials; Power; Electrical conductivity
Citation Formats
Luo, Zhong-Zhen, Hao, Shiqiang, Cai, Songting, Bailey, Trevor P., Tan, Gangjian, Luo, Yubo, Spanopoulos, Ioannis, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., Yan, Qingyu, and Kanatzidis, Mercouri G. Enhancement of Thermoelectric Performance for n-Type PbS through Synergy of Gap State and Fermi Level Pinning. United States: N. p., 2019.
Web. doi:10.1021/jacs.9b01889.
Luo, Zhong-Zhen, Hao, Shiqiang, Cai, Songting, Bailey, Trevor P., Tan, Gangjian, Luo, Yubo, Spanopoulos, Ioannis, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., Yan, Qingyu, & Kanatzidis, Mercouri G. Enhancement of Thermoelectric Performance for n-Type PbS through Synergy of Gap State and Fermi Level Pinning. United States. https://doi.org/10.1021/jacs.9b01889
Luo, Zhong-Zhen, Hao, Shiqiang, Cai, Songting, Bailey, Trevor P., Tan, Gangjian, Luo, Yubo, Spanopoulos, Ioannis, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., Yan, Qingyu, and Kanatzidis, Mercouri G. Wed .
"Enhancement of Thermoelectric Performance for n-Type PbS through Synergy of Gap State and Fermi Level Pinning". United States. https://doi.org/10.1021/jacs.9b01889. https://www.osti.gov/servlets/purl/1777108.
@article{osti_1777108,
title = {Enhancement of Thermoelectric Performance for n-Type PbS through Synergy of Gap State and Fermi Level Pinning},
author = {Luo, Zhong-Zhen and Hao, Shiqiang and Cai, Songting and Bailey, Trevor P. and Tan, Gangjian and Luo, Yubo and Spanopoulos, Ioannis and Uher, Ctirad and Wolverton, Chris and Dravid, Vinayak P. and Yan, Qingyu and Kanatzidis, Mercouri G.},
abstractNote = {In this paper, we report that Ga-doped and Ga-In-codoped n-type PbS samples show excellent thermoelectric performance in the intermediate temperature range. First-principles electronic structure calculations reveal that Ga doping can cause Fermi level pinning in PbS by introducing a gap state between the conduction and valence bands. Furthermore, Ga-In codoping introduces an extra conduction band. These added electronic features lead to high electron mobilities up to μH ~ 630 cm2 V-1 s-1 for n of 1.67 × 1019 cm-3 and significantly enhanced Seebeck coefficients in PbS. Consequently, we obtained a maximum power factor of ~32 μW cm-1 K-2 at 300 K for Pb0.9875Ga0.0125S, which is the highest reported for PbS-based systems giving a room-temperature figure of merit, ZT, of ~0.35 and ~0.82 at 923 K. For the codoped Pb0.9865Ga0.0125In0.001S, the maximum ZT rises to ~1.0 at 923 K and achieves a record-high average ZT (ZTavg) of ~0.74 in the temperature range of 400-923 K.},
doi = {10.1021/jacs.9b01889},
journal = {Journal of the American Chemical Society},
number = 15,
volume = 141,
place = {United States},
year = {Wed Mar 27 00:00:00 EDT 2019},
month = {Wed Mar 27 00:00:00 EDT 2019}
}
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