Soft phonon modes from off-center Ge atoms lead to ultralow thermal conductivity and superior thermoelectric performance in n-type PbSe–GeSe
Abstract
Historically PbSe has underperformed PbTe in thermoelectric efficiency and has been regarded as an inferior relative to its telluride congener. However, the fifty-fold greater natural abundance of Se relative to Te makes PbSe appealing as a thermoelectric material. We report that the n-type GeSe-alloyed PbSe system achieves a peak figure of merit, ZT, of ~1.54 at 773 K and maintains ZT values above 1.2 over a broad temperature range from 623 K to 923 K. The highest performing composition is Sb-doped PbSe–12%GeSe, which exhibits an ultralow lattice thermal conductivity of ~0.36 W m–1 K–1 at 573 K, close to the limit of amorphous PbSe. Theoretical studies reveal that the alloyed Ge2+ atoms prefer to stay at off-center lattice positions, inducing low frequency modes. The Ge atoms also cause the unexpected behavior where the next nearest atom neighbors (6 Pb atoms) oscillate at lower frequencies than in pure PbSe leading to a large reduction of the Debye temperature and acoustic phonon velocity. The Pb0.9955Sb0.0045Se–12%GeSe system also shows Ge-rich precipitates and many aligned dislocations within its microstructure which also contribute to phonon scattering. The resultant average ZT (ZTavg), a broad measure of the material's potential for functional thermoelectric modules, is 1.06 frommore »
- Authors:
-
[1];
[2];
[2];
[2];
[3];
[3];
[2];
[2];
[4];
[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)
- 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); Singapore MOE AcRF Tier 1
- OSTI Identifier:
- 1775350
- Alternate Identifier(s):
- OSTI ID: 1467542
- Grant/Contract Number:
- SC0014520; AC02-06CH11357; AC02-05CH11231; 2016-T1-002-065
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy & Environmental Science
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 11; Journal ID: ISSN 1754-5692
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Luo, Zhong-Zhen, Hao, Shiqiang, Zhang, Xiaomi, Hua, Xia, Cai, Songting, Tan, Gangjian, Bailey, Trevor P., Ma, Runchu, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., Yan, Qingyu, and Kanatzidis, Mercouri G. Soft phonon modes from off-center Ge atoms lead to ultralow thermal conductivity and superior thermoelectric performance in n-type PbSe–GeSe. United States: N. p., 2018.
Web. doi:10.1039/c8ee01755g.
Luo, Zhong-Zhen, Hao, Shiqiang, Zhang, Xiaomi, Hua, Xia, Cai, Songting, Tan, Gangjian, Bailey, Trevor P., Ma, Runchu, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., Yan, Qingyu, & Kanatzidis, Mercouri G. Soft phonon modes from off-center Ge atoms lead to ultralow thermal conductivity and superior thermoelectric performance in n-type PbSe–GeSe. United States. https://doi.org/10.1039/c8ee01755g
Luo, Zhong-Zhen, Hao, Shiqiang, Zhang, Xiaomi, Hua, Xia, Cai, Songting, Tan, Gangjian, Bailey, Trevor P., Ma, Runchu, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., Yan, Qingyu, and Kanatzidis, Mercouri G. Mon .
"Soft phonon modes from off-center Ge atoms lead to ultralow thermal conductivity and superior thermoelectric performance in n-type PbSe–GeSe". United States. https://doi.org/10.1039/c8ee01755g. https://www.osti.gov/servlets/purl/1775350.
@article{osti_1775350,
title = {Soft phonon modes from off-center Ge atoms lead to ultralow thermal conductivity and superior thermoelectric performance in n-type PbSe–GeSe},
author = {Luo, Zhong-Zhen and Hao, Shiqiang and Zhang, Xiaomi and Hua, Xia and Cai, Songting and Tan, Gangjian and Bailey, Trevor P. and Ma, Runchu and Uher, Ctirad and Wolverton, Chris and Dravid, Vinayak P. and Yan, Qingyu and Kanatzidis, Mercouri G.},
abstractNote = {Historically PbSe has underperformed PbTe in thermoelectric efficiency and has been regarded as an inferior relative to its telluride congener. However, the fifty-fold greater natural abundance of Se relative to Te makes PbSe appealing as a thermoelectric material. We report that the n-type GeSe-alloyed PbSe system achieves a peak figure of merit, ZT, of ~1.54 at 773 K and maintains ZT values above 1.2 over a broad temperature range from 623 K to 923 K. The highest performing composition is Sb-doped PbSe–12%GeSe, which exhibits an ultralow lattice thermal conductivity of ~0.36 W m–1 K–1 at 573 K, close to the limit of amorphous PbSe. Theoretical studies reveal that the alloyed Ge2+ atoms prefer to stay at off-center lattice positions, inducing low frequency modes. The Ge atoms also cause the unexpected behavior where the next nearest atom neighbors (6 Pb atoms) oscillate at lower frequencies than in pure PbSe leading to a large reduction of the Debye temperature and acoustic phonon velocity. The Pb0.9955Sb0.0045Se–12%GeSe system also shows Ge-rich precipitates and many aligned dislocations within its microstructure which also contribute to phonon scattering. The resultant average ZT (ZTavg), a broad measure of the material's potential for functional thermoelectric modules, is 1.06 from 400 K to 800 K, the highest among all previously reported n- and p-type PbSe. Furthermore, this value matches or exceeds even those of the best n-type PbTe-based thermoelectric materials.},
doi = {10.1039/c8ee01755g},
journal = {Energy & Environmental Science},
number = 11,
volume = 11,
place = {United States},
year = {Mon Aug 13 00:00:00 EDT 2018},
month = {Mon Aug 13 00:00:00 EDT 2018}
}
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