High Thermoelectric Performance in PbSe–NaSbSe2 Alloys from Valence Band Convergence and Low Thermal Conductivity

Tyler J. Slade, Trevor P. Bailey, Jann A. Grovogui, Xia Hua, Xiaomi Zhang, Jimmy Jiahong Kuo, Ido Hadar, G. Jeffrey Snyder, Chris Wolverton, Vinayak P. Dravid, Ctirad Uher, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

Abstract

PbSe is an attractive thermoelectric material due to its favorable electronic structure, high melting point, and lower cost compared to PbTe. Herein, the hitherto unexplored alloys of PbSe with NaSbSe2 (NaPbmSbSem+2) are described and the most promising p-type PbSe-based thermoelectrics are found among them. Surprisingly, it is observed that below 500 K, NaPbmSbSem+2 exhibits unorthodox semiconducting-like electrical conductivity, despite possessing degenerate carrier densities of ≈1020 cm−3. It is shown that the peculiar behavior derives from carrier scattering by the grain boundaries. It is further demonstrated that the high solubility of NaSbSe2 in PbSe augments both the thermoelectric properties while maintaining a rock salt structure. Namely, density functional theory calculations and photoemission spectroscopy demonstrate that introduction of NaSbSe2 lowers the energy separation between the L- and Σ-valence bands and enhances the power factors under 700 K. The crystallographic disorder of Na+, Pb2+, and Sb3+ moreover provides exceptionally strong point defect phonon scattering yielding low lattice thermal conductivities of 1–0.55 W m-1 K-1 between 400 and 873 K without nanostructures. As a consequence, NaPb10SbSe12 achieves maximum ZT ≈1.4 near 900 K when optimally doped. More importantly, NaPb10SbSe12 maintains high ZT across a broad temperature range, giving an estimated record ZTavg of ≈0.64 between 400 and 873 K, a significant improvement over existing p-type PbSe thermoelectrics.

Original languageEnglish
Article number1901377
JournalAdvanced Energy Materials
DOIs
Publication statusPublished - Jan 1 2019

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Phonon scattering
Point defects
Photoelectron spectroscopy
Valence bands
Crystal lattices
Electronic structure
Density functional theory
Carrier concentration
Melting point
Nanostructures
Thermal conductivity
Grain boundaries
Solubility
Rocks
Scattering
Salts
Costs
Temperature
Electric Conductivity
lead selenide

Keywords

  • band structure engineering
  • grain boundary charge transport
  • low thermal conductivity
  • PbSe alloying
  • thermoelectric materials

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

Cite this

High Thermoelectric Performance in PbSe–NaSbSe2 Alloys from Valence Band Convergence and Low Thermal Conductivity. / Slade, Tyler J.; Bailey, Trevor P.; Grovogui, Jann A.; Hua, Xia; Zhang, Xiaomi; Kuo, Jimmy Jiahong; Hadar, Ido; Snyder, G. Jeffrey; Wolverton, Chris; Dravid, Vinayak P.; Uher, Ctirad; Kanatzidis, Mercouri G.

In: Advanced Energy Materials, 01.01.2019.

Research output: Contribution to journalArticle

Slade, TJ, Bailey, TP, Grovogui, JA, Hua, X, Zhang, X, Kuo, JJ, Hadar, I, Snyder, GJ, Wolverton, C, Dravid, VP, Uher, C & Kanatzidis, MG 2019, 'High Thermoelectric Performance in PbSe–NaSbSe2 Alloys from Valence Band Convergence and Low Thermal Conductivity', Advanced Energy Materials. https://doi.org/10.1002/aenm.201901377
Slade, Tyler J. ; Bailey, Trevor P. ; Grovogui, Jann A. ; Hua, Xia ; Zhang, Xiaomi ; Kuo, Jimmy Jiahong ; Hadar, Ido ; Snyder, G. Jeffrey ; Wolverton, Chris ; Dravid, Vinayak P. ; Uher, Ctirad ; Kanatzidis, Mercouri G. / High Thermoelectric Performance in PbSe–NaSbSe2 Alloys from Valence Band Convergence and Low Thermal Conductivity. In: Advanced Energy Materials. 2019.
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AU - Zhang, Xiaomi

AU - Kuo, Jimmy Jiahong

AU - Hadar, Ido

AU - Snyder, G. Jeffrey

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AU - Dravid, Vinayak P.

AU - Uher, Ctirad

AU - Kanatzidis, Mercouri G

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