ABa6Cu31Te22 (A = K, Rb, Cs) Featuring Polyanionic Copper–Telluride Frameworks with Ultralow Thermal Conductivity

Sarkar, Arka; Cerasoli, Frank T.; Viswanathan, Gayatri; Donadio, Davide; Kovnir, Kirill

doi:10.1021/acsami.4c06694

Title: ABa₆Cu₃₁Te₂₂ (A = K, Rb, Cs) Featuring Polyanionic Copper–Telluride Frameworks with Ultralow Thermal Conductivity

Journal Article · Tue Jul 16 00:00:00 UTC 2024 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.4c06694 · OSTI ID:2434324

Sarkar, Arka ^[1]; Cerasoli, Frank T. ^[2];

^[1];

^[2];

^[1]

Ames Laboratory (AMES), Ames, IA (United States); Iowa State University, Ames, IA (United States)
University of California, Davis, CA (United States)

In this study, hree polyanionic tellurides, ABa₆Cu₃₁Te₂₂ (A = K, Rb, Cs), were synthesized in salt flux. The isostructural tellurides crystallize in a new structure type, in the cubic Pa$$\overline{3}$$ space group with a Wyckoff sequence of d¹⁰c²b¹ and large unit cell volumes of over 5500 Å³. The structures feature a framework of [CuTe₄] tetrahedra and [CuTe₃] trigonal pyramids with disorder in the Cu sites. The polyanionic frameworks have large square antiprism and cuboctahedral voids where Ba and alkali metal cations are situated, forming [BaTe₈] and [ATe₁₂], respectively. The overall compositions are close to being charge balanced. The large [ATe₁₂] cuboctahedra allowed for significant anisotropic displacement of the A cations, as observed from both single crystal X-ray diffraction and heat capacity studies. Alkali cations rattling together with Cu atom displacement and disorder leads to the dispersion of phonons, thus softening the lattice and subsequently reducing the thermal conductivity. Evaluations of the electronic band structure revealed the occurrence of a narrow bandgap together with the presence of a flat band near the valence band maximum, giving rise to the high thermopower. The Cs and Rb analogues show a slope change in the temperature dependence of electrical resistivity around room temperature, which is typical for semimetals or degenerate semiconductors. For the as-synthesized and unoptimized materials, high values of the thermoelectric figure-of-merit of ~0.2 were observed at 623 K.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

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

Grant/Contract Number:: AC02-07CH11358; SC0022288

OSTI ID:: 2434324

Report Number(s):: IS-J--11,387

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 30 Vol. 16; ISSN 1944-8244

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
anharmonicity
crystal structure
disorder
framework
thermal conductivity
thermoelectric

Title: ABa6Cu31Te22 (A = K, Rb, Cs) Featuring Polyanionic Copper–Telluride Frameworks with Ultralow Thermal Conductivity

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Title: ABa₆Cu₃₁Te₂₂ (A = K, Rb, Cs) Featuring Polyanionic Copper–Telluride Frameworks with Ultralow Thermal Conductivity