Chemical Insights into PbSe–x%HgSe: High Power Factor and Improved Thermoelectric Performance by Alloying with Discordant Atoms

Hodges, James M.; Hao, Shiqiang; Grovogui, Jann A.; Zhang, Xiaomi; Bailey, Trevor P.; Li, Xiang; Gan, Zhehong; Hu, Yan-Yan; Uher, Ctirad; Dravid, Vinayak P.; Wolverton, Chris; Kanatzidis, Mercouri G.

doi:10.1021/jacs.8b11050

Title: Chemical Insights into PbSe–x%HgSe: High Power Factor and Improved Thermoelectric Performance by Alloying with Discordant Atoms

Journal Article · Wed Nov 21 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b11050· OSTI ID:1612226

Hodges, James M. ^[1]; Hao, Shiqiang ^[1]; Grovogui, Jann A. ^[1]; Zhang, Xiaomi ^[1]; Bailey, Trevor P. ^[2]; Li, Xiang ^[3]; Gan, Zhehong ^[4];

^[5]; Uher, Ctirad ^[2];

^[1];

^[1]

Northwestern University, Evanston, IL (United States)
University of Michigan, Ann Arbor, MI (United States)
Florida State University, Tallahassee, FL (United States)
National High Magnetic Field Laboratory, Tallahassee, FL (United States)
Florida State University, Tallahassee, FL (United States); National High Magnetic Field Laboratory, Tallahassee, FL (United States)

Thermoelectric generators can convert heat directly into usable electric power but suffer from low efficiencies and high costs, which have hindered wide-scale applications. Accordingly, an important goal in the field of thermoelectricity is to develop new high performance materials that are composed of more earth-abundant elements. The best systems for midtemperature power generation rely on heavily doped PbTe, but the Te in these materials is scarce in the Earth’s crust. PbSe is emerging as a less expensive alternative to PbTe, although it displays inferior performance due to a considerably smaller power factor S²σ, where S is the Seebeck coefficient and σ is electrical conductivity. In this report we present a new p-type PbSe system, Pb_0.98Na_0.02Se–x%HgSe, which yields a very high power factor of ~20 μW·cm^–1·K^–2 at 963 K when x = 2, a 15% improvement over the best performing PbSe–x%MSe materials. The enhancement is attributed to a combination of high carrier mobility and the early onset of band convergence in the Hg-alloyed samples (~550 K), which results in a significant increase in the Seebeck coefficient. Interestingly, we find that the Hg²⁺ cations sit at an off-centered position within the PbSe lattice, and we dub the displaced Hg atoms “discordant”. DFT calculations indicate that this feature plays a role in lowering thermal conductivity, and we believe that this insight may inspire new design criteria for engineering high performance thermoelectric materials. The high power factor combined with a decrease in thermal conductivity gives a high figure of merit ZT of 1.7 at 970 K, the highest value reported for p-type PbSe to date.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF); Keck Foundation; State of Illinois

Grant/Contract Number:: SC0014520; AC02-05CH11231; AC02-06CH11357; ECCS-1542205; DMR-1720139; DGE-1324585

OSTI ID:: 1612226

Journal Information:: Journal of the American Chemical Society, Vol. 140, Issue 51; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 64 works

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