Low Thermal Conductivity in Heteroanionic Materials with Layers of Homoleptic Polyhedra

Zhang, Chi; He, Jiangang; McClain, Rebecca; Xie, Hongyao; Cai, Songting; Walters, Lauren N.; Shen, Jiahong; Ding, Fenghua; Zhou, Xiuquan; Malliakas, Christos D.; Rondinelli, James M.; Kanatzidis, Mercouri G.; Wolverton, Chris; Dravid, Vinayak P.; Poeppelmeier, Kenneth R.

doi:10.1021/jacs.1c10284

Title: Low Thermal Conductivity in Heteroanionic Materials with Layers of Homoleptic Polyhedra

Journal Article · 03 February 2022 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.1c10284 · OSTI ID:1863390

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Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Although BiAgOSe, an analogue of a well-studied thermoelectric material BiCuOSe, is thermodynamically stable, its synthesis is complicated by the low driving force of formation from the stable binary and ternary intermediates. Here we have developed a “subtraction strategy” to suppress byproducts and produce pure phase BiAgOSe using hydrothermal methods. Electronic structure calculations and optical characterization show that BiAgOSe is an indirect bandgap semiconductor with a bandgap of 0.95 eV. The prepared sample exhibits lower lattice thermal conductivities (0.61 W·m^–1·K^–1 at room temperature and 0.35 W·m^–1·K^–1 at 650 K) than BiCuOSe. Further, lattice dynamical simulations and variable temperature diffraction measurements demonstrate that the low lattice thermal conductivity arises from both the low sound velocity and high phonon–phonon scattering rates in BiAgOSe. These in turn result primarily from the soft Ag–Se bonds in the edge-sharing AgSe₄ tetrahedra and large sublattice mismatch between the quasi-two-dimensional [Bi₂O₂]²⁺ and [Ag₂Se₂]^2– layers. These results highlight the advantages of manipulating the chemistry of homoleptic polyhedra in heteroanionic compounds for electronic structure and phonon transport control.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0014520

OSTI ID:: 1863390

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 6 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Diffraction
Lattices
Layers
Phonons
Thermal conductivity

Title: Low Thermal Conductivity in Heteroanionic Materials with Layers of Homoleptic Polyhedra

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