Abstract
The gallium composition dependence of crystallographic and thermoelectric properties in polycrystalline n-type Ba8GaxSi46−x (nominal x=14–18) compounds with the type-I clathrate structure is presented. Samples were prepared by combining arc melting and spark plasma sintering methods. Powder x-ray diffraction, Rietveld analysis, scanning electron microscopy, and energy-dispersive x-ray spectroscopy show that the solubility limit of gallium in the type-I clathrate phase is close to x=15, which is slightly higher than that for a single crystal. The carrier concentration at room temperature decreases from 2×1021cm−3 to 4×1020cm−3 as the Ga content x increases. The Seebeck coefficient, the electrical conductivity, and the thermal conductivity vary systematically with the carrier concentration when the Ga content x varies. The effective mass (2.0m0), the carrier mobility (10cm2V−1s−1), and the lattice thermal conductivity (1.1Wm−1K−1) are determined for the Ga content x=14.51. The dimensionless thermoelectric figure of merit ZT is about 0.55 at 900K for the Ga content x=14.51. The calculation of ZT using the experimentally determined material parameters predicts ZT=0.8 (900K) at the optimum carrier concentration of about 2×1020cm−3.
Published Version
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