Systematic over-estimation of lattice thermal conductivity in materials with electrically-resistive grain boundaries

Kuo, Jimmy Jiahong; Wood, Max; Slade, Tyler J.; Kanatzidis, Mercouri G.; Snyder, G. Jeffrey

doi:10.1039/c9ee03921j

Systematic over-estimation of lattice thermal conductivity in materials with electrically-resistive grain boundaries

Journal Article · Tue Feb 25 00:00:00 EST 2020 · Energy & Environmental Science

DOI:https://doi.org/10.1039/c9ee03921j· OSTI ID:1777414

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Northwestern Univ., Evanston, IL (United States); Northwestern University
Northwestern Univ., Evanston, IL (United States)

Reducing the thermal conductivity κ of a material via nano-structuring to create small grain sizes is one of the most common strategies to improve thermoelectric materials. In such polycrystalline materials heat carrying phonons are scattered at the grain boundaries, which directly improves the thermoelectric quality factor and ultimately the figure-of-merit zT. In some cases, however, such as in Mg₃Sb₂, SnSe, and Mg₂Si an opposite trend is found where higher lattice thermal conductivity reported in small grain polycrystalline material than in large grain or single crystal materials. This unphysical result indicates a problem with the conventional use of the Wiedemann–Franz law. Here, we trace this problematic finding to the electrical resistance at the grain boundaries, which leads to an overestimation of the phonon or lattice contribution of the thermal conductivity κ_L. In materials with significant grain boundary electrical resistance, the estimated electronic contribution to the thermal conductivity LσT is low because the measured electrical conductivity σ is low. However within the grain electrons may still be transporting more heat than the total conductivity suggests, leading to an overestimation of κ_L if the conventional κ_L = κ – LσT is used with the measured values of κ and σ. Here, the overestimation of κL in small-grain samples is shown to be pervasive across a broad range of thermoelectric materials, including Mg₃Sb₂, Mg₂Si, PbTe, PbSe, SnSe, (Hf,Zr)CoSb, CoSb₃, and Bi₂Te₃ alloys, and a correction is necessary to properly understand and predict their charge and heat transport.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0014520

OSTI ID:: 1777414

Alternate ID(s):: OSTI ID: 1602570

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 4 Vol. 13; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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