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.

doi:10.1002/aenm.201901377

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

Journal Article · Mon Jul 01 00:00:00 EDT 2019 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201901377· OSTI ID:1777259

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Northwestern Univ., Evanston, IL (United States); Northwestern University
Univ. of Michigan, Ann Arbor, MI (United States)
Northwestern Univ., Evanston, IL (United States)

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 (NaPb_mSbSe_m+2) are described and the most promising p-type PbSe-based thermoelectrics are found among them. Surprisingly, it is observed that below 500 K, NaPb_mSbSe_m+2 exhibits unorthodox semiconducting-like electrical conductivity, despite possessing degenerate carrier densities of ≈10²⁰ cm^-3. Here, 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 ZT_avg of ≈0.64 between 400 and 873 K, a significant improvement over existing p-type PbSe thermoelectrics.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: National Science Foundation Graduate Research Fellowship; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0014520

OSTI ID:: 1777259

Alternate ID(s):: OSTI ID: 1612214
OSTI ID: 1530472

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 30 Vol. 9; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
PbSe alloying
band structure engineering
grain boundary charge transport
low thermal conductivity
thermoelectric materials