Tuning Thermoelectric Properties of Type I Clathrate K8–xBaxAl8+xSi38–x through Barium Substitution

Sui, Fan; Kauzlarich, Susan M.

doi:10.1021/acs.chemmater.6b00566

Title: Tuning Thermoelectric Properties of Type I Clathrate K_8–xBa_xAl_8+xSi_38–x through Barium Substitution

Journal Article · Wed Apr 20 00:00:00 EDT 2016 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.6b00566· OSTI ID:1248407

Sui, Fan ^[1]; Kauzlarich, Susan M. ^[1]

Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States

The thermal stability and thermoelectric properties of type I clathrate K₈Al₈Si₃₈ up to 873 K are reported. K₈Al₈Si₃₈ possesses a high absolute Seebeck coefficient value and high electrical resistivity in the temperature range of 323 to 873 K, which is consistent with previously reported low temperature thermoelectric properties. Samples with Ba partial substitution at the K guest atom sites were synthesized from metal hydride precursors. The samples with the nominal chemical formula of K_8–xBa_xAl_8+xSi_38–x (x = 1, 1.5, 2) possess type I clathrate structure (cubic, Pm3¯n), confirmed by X-ray diffraction. The guest atom site occupancies and thermal motions were investigated with Rietveld refinement of synchrotron powder X-ray diffraction. Transport properties of Ba-containing samples were characterized from 2 to 300 K. The K–Ba alloy phases showed low thermal conductivity and improved electrical conductivity compared to K₈Al₈Si₃₈. Electrical resistivity and Seebeck coefficients were measured over the temperature range of 323 to 873 K. Thermal conductivity from 323 to 873 K was estimated from the Wiedemann–Franz relation and lattice thermal conductivity extrapolation from 300 to 873 K. K_8–xBa_xAl_8+xSi_38–x (x = 1, 1.5) synthesized with Al deficiency showed enhanced electrical conductivity, and the absolute Seebeck coefficients decrease with the increased carrier concentration. When x = 2, the Al content increases toward the electron balanced composition, and the electrical resistivity increases with the decreasing charge carrier concentration. Overall, K_6.5Ba_1.5Al₉Si₃₇ achieves an enhanced zT of 0.4 at 873 K.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

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

Grant/Contract Number:: DMR-1405973; AC02-06CH11357

OSTI ID:: 1248407

Alternate ID(s):: OSTI ID: 1322345

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Vol. 28 Journal Issue: 9; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 20 works

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thermal conductivity
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Title: Tuning Thermoelectric Properties of Type I Clathrate K8–xBaxAl8+xSi38–x through Barium Substitution

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Title: Tuning Thermoelectric Properties of Type I Clathrate K_8–xBa_xAl_8+xSi_38–x through Barium Substitution