Lone-Electron-Pair Micelles Strengthen Bond Anharmonicity in MnPb16Sb14S38 Complex Sulfosalt Leading to Ultra-Low Thermal Conductivity

Dawahre, Lamia; Lu, Ruiming; Djieutedjeu, Honore; Lopez, Juan S.; Bailey, Trevor P.; Buchanan, Brandon; Yin, Zhixiong; Uher, Ctirad; Poudeu, Pierre F. P.

doi:10.1021/acsami.0c12938

Title: Lone-Electron-Pair Micelles Strengthen Bond Anharmonicity in MnPb16Sb14S38 Complex Sulfosalt Leading to Ultra-Low Thermal Conductivity

Journal Article · Wed Sep 09 00:00:00 EDT 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c12938· OSTI ID:1659383

Dawahre, Lamia ^[1]; Lu, Ruiming ^[1]; Djieutedjeu, Honore ^[1]; Lopez, Juan S. ^[1]; Bailey, Trevor P. ^[1]; Buchanan, Brandon ^[1]; Yin, Zhixiong ^[1]; Uher, Ctirad ^[1]; Poudeu, Pierre F. P. ^[1]

University of Michigan, Ann Arbor, MI (United States)

Designing crystalline solids in which intrinsic extremely low lattice thermal conductivity mainly arises from its unique bonding nature rather than structure complexity and/or atomic disorder could promote thermal energy manipulation and utilization for applications ranging from thermoelectric energy conversion to thermal barrier coatings. Here, we report an extremely low lattice thermal conductivity of ~0.34 W m-1 K-1 at 300 K in the new complex sulfosalt MnPb16Sb14S38. We attribute the ultra-low lattice thermal conductivity to a synergistic combination of scattering mechanisms involving (1) strong bond anharmonicity in various structural building units, owing to the presence of stereoactive lone-electron-pair (LEP) micelles, and (2) phonon scattering at the interfaces between building units of increasing size and complexity. Remarkably, low-temperature heat capacity measurement revealed a Cp value of 0.206 J g-1 K-1 at T > 300 K, which is 22% lower than the Dulong-Petit value (0.274 J g-1 K-1). Further analysis of the Cp data and sound velocity (ν = 1834 m/s) measurement yielded Debye temperature values of 161 K and 187 K, respectively. Here, the resulting Grüneisen parameter, γ = 1.65, further supports strong bond anharmonicity as the dominant mechanism responsible for the observed extremely low lattice thermal conductivity.

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Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

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

Grant/Contract Number:: SC0018941; DMR-1428226; CHE-104008

OSTI ID:: 1659383

Journal Information:: ACS Applied Materials and Interfaces, Vol. 12, Issue 40; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Lone-Electron-Pair Micelles Strengthen Bond Anharmonicity in MnPb16Sb14S38 Complex Sulfosalt Leading to Ultra-Low Thermal Conductivity

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