Soft phonon modes from off-center Ge atoms lead to ultralow thermal conductivity and superior thermoelectric performance in n-type PbSe–GeSe
Journal Article
·
· Energy & Environmental Science
- Nanyang Technological Univ. (Singapore); Northwestern Univ., Evanston, IL (United States); Northwestern University
- Northwestern Univ., Evanston, IL (United States)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Nanyang Technological Univ. (Singapore)
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.
- Research Organization:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Organization:
- Singapore MOE AcRF Tier 1; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- AC02-05CH11231; AC02-06CH11357; SC0014520
- OSTI ID:
- 1775350
- Alternate ID(s):
- OSTI ID: 1467542
- Journal Information:
- Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 11 Vol. 11; ISSN 1754-5692
- Publisher:
- Royal Society of ChemistryCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Similar Records
High Figure of Merit in Gallium-Doped Nanostructured n-Type PbTe-xGeTe with Midgap States
Chemical Insights into PbSe–x%HgSe: High Power Factor and Improved Thermoelectric Performance by Alloying with Discordant Atoms
Valence Disproportionation of GeS in the PbS Matrix Forms Pb5Ge5S12 Inclusions with Conduction Band Alignment Leading to High n-Type Thermoelectric Performance
Journal Article
·
Tue Sep 10 20:00:00 EDT 2019
· Journal of the American Chemical Society
·
OSTI ID:1776870
Chemical Insights into PbSe–x%HgSe: High Power Factor and Improved Thermoelectric Performance by Alloying with Discordant Atoms
Journal Article
·
Tue Nov 20 19:00:00 EST 2018
· Journal of the American Chemical Society
·
OSTI ID:1612226
Valence Disproportionation of GeS in the PbS Matrix Forms Pb5Ge5S12 Inclusions with Conduction Band Alignment Leading to High n-Type Thermoelectric Performance
Journal Article
·
Wed Apr 13 20:00:00 EDT 2022
· Journal of the American Chemical Society
·
OSTI ID:1867609