Improved thermoelectric performance in Yb14Mn 1-xZnxSb11 by the reduction of spin-disorder scattering

Shawna R. Brown, Eric S. Toberer, Teruyuki Ikeda, Catherine A. Cox, Franck Gascoin, Susan M. Kauzlarich, G. Jeffrey Snyder

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Abstract

Rare-earth transition metal compounds Yb14Mn 1-xZnx,Sb11, isostructural with Ca 14AlSb11, have been prepared using a metal flux growth technique for thermoelectric property measurements (with x = 0.0, 0.2, 0.3, 0.4, 0.7, 0.9, and 1.0). Single-crystal X-ray diffraction and electron microprobe analysis data indicate the successful synthesis of a solid-solution for the Yb14Mn1-xZnxSb11 structure type for 0< x < 0.4. Hot-pressed polycrystalline samples showed that the product from the flux reaction was a pure phase from x = 0 through x = 0.4 with the presence of a minor secondary phase for compositions x > 0.4. High-temperature (298 K-1275 K) measurements of the Seebeck coefficient, resistivity, and thermal conductivity were performed on hot-pressed, polycrystalline samples. As the concentration of Zn increases in Yb 14Mn1-xZnxSb11, the Seebeck coefficient remains unchanged for 0 ≤ x ≤ 0.7 indicating that the free carrier concentration has remained unchanged. However, as the nonmagnetic Zn2+ ions replace the magnetic Mn2+ ions, the spin disorder scattering is reduced, lowering the resistivity. Replacing the magnetic Mn2+ with non magnetic Zn2+ provides an independent means to lower resistivity without deleterious effects to the Seebeck values or thermal conduction. Alloying the Mn site with Zn reduces the lattice thermal conductivity at low temperatures but has negligible impact at high temperatures. The reduction of spin disorder scattering leads to an ̃10% improvement over Yb14MnSb11, revealing a maximum thermoelectric figure of merit (zT) of ̃1.1 at 1275 K for Yb14Mn0.6Zn 0.4Sb11.

Original languageEnglish (US)
Pages (from-to)3412-3419
Number of pages8
JournalChemistry of Materials
Volume20
Issue number10
DOIs
StatePublished - May 27 2008

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Seebeck coefficient
Scattering
Thermal conductivity
Transition metal compounds
Ions
Electron probe microanalysis
Alloying
Temperature
Rare earths
Carrier concentration
Solid solutions
Metals
Single crystals
Fluxes
X ray diffraction
Hot Temperature

ASJC Scopus subject areas

  • Materials Chemistry
  • Materials Science(all)

Cite this

Brown, S. R., Toberer, E. S., Ikeda, T., Cox, C. A., Gascoin, F., Kauzlarich, S. M., & Snyder, G. J. (2008). Improved thermoelectric performance in Yb14Mn 1-xZnxSb11 by the reduction of spin-disorder scattering. Chemistry of Materials, 20(10), 3412-3419. https://doi.org/10.1021/cm703616q

Improved thermoelectric performance in Yb14Mn 1-xZnxSb11 by the reduction of spin-disorder scattering. / Brown, Shawna R.; Toberer, Eric S.; Ikeda, Teruyuki; Cox, Catherine A.; Gascoin, Franck; Kauzlarich, Susan M.; Snyder, G. Jeffrey.

In: Chemistry of Materials, Vol. 20, No. 10, 27.05.2008, p. 3412-3419.

Research output: Contribution to journalArticle

Brown, SR, Toberer, ES, Ikeda, T, Cox, CA, Gascoin, F, Kauzlarich, SM & Snyder, GJ 2008, 'Improved thermoelectric performance in Yb14Mn 1-xZnxSb11 by the reduction of spin-disorder scattering', Chemistry of Materials, vol. 20, no. 10, pp. 3412-3419. https://doi.org/10.1021/cm703616q
Brown SR, Toberer ES, Ikeda T, Cox CA, Gascoin F, Kauzlarich SM et al. Improved thermoelectric performance in Yb14Mn 1-xZnxSb11 by the reduction of spin-disorder scattering. Chemistry of Materials. 2008 May 27;20(10):3412-3419. https://doi.org/10.1021/cm703616q
Brown, Shawna R. ; Toberer, Eric S. ; Ikeda, Teruyuki ; Cox, Catherine A. ; Gascoin, Franck ; Kauzlarich, Susan M. ; Snyder, G. Jeffrey. / Improved thermoelectric performance in Yb14Mn 1-xZnxSb11 by the reduction of spin-disorder scattering. In: Chemistry of Materials. 2008 ; Vol. 20, No. 10. pp. 3412-3419.
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AB - Rare-earth transition metal compounds Yb14Mn 1-xZnx,Sb11, isostructural with Ca 14AlSb11, have been prepared using a metal flux growth technique for thermoelectric property measurements (with x = 0.0, 0.2, 0.3, 0.4, 0.7, 0.9, and 1.0). Single-crystal X-ray diffraction and electron microprobe analysis data indicate the successful synthesis of a solid-solution for the Yb14Mn1-xZnxSb11 structure type for 0< x < 0.4. Hot-pressed polycrystalline samples showed that the product from the flux reaction was a pure phase from x = 0 through x = 0.4 with the presence of a minor secondary phase for compositions x > 0.4. High-temperature (298 K-1275 K) measurements of the Seebeck coefficient, resistivity, and thermal conductivity were performed on hot-pressed, polycrystalline samples. As the concentration of Zn increases in Yb 14Mn1-xZnxSb11, the Seebeck coefficient remains unchanged for 0 ≤ x ≤ 0.7 indicating that the free carrier concentration has remained unchanged. However, as the nonmagnetic Zn2+ ions replace the magnetic Mn2+ ions, the spin disorder scattering is reduced, lowering the resistivity. Replacing the magnetic Mn2+ with non magnetic Zn2+ provides an independent means to lower resistivity without deleterious effects to the Seebeck values or thermal conduction. Alloying the Mn site with Zn reduces the lattice thermal conductivity at low temperatures but has negligible impact at high temperatures. The reduction of spin disorder scattering leads to an ̃10% improvement over Yb14MnSb11, revealing a maximum thermoelectric figure of merit (zT) of ̃1.1 at 1275 K for Yb14Mn0.6Zn 0.4Sb11.

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