Abstract
Polycrystalline thermoelectric Co1−xMxSb3 (M=Ni, Pd) skutterudites have been synthesized by melting, annealing, and spark plasma sintering. The solubility limit of Pd and Ni are determined to be respectively xmax=0.03 and xmax=0.09. The density of states effective masses range between 2.0m0 and 4m0 in Co1−xPdxSb3 and Co1−xNixSb3. These values are consistent with the effective band mass (0.3m0) and the degeneracy number Nv=36 derived from band structure calculations. Power factor measurements and calculations in Co1−xPdxSb3 show that at 300K, the optimum electron concentration would be [n]opt=1.4×1020cm−3, slightly beyond the electron concentration (1.1×1020cm−3) of the solubility limit composition Co0.97Pd0.03Sb3. The maximum power factor is effectively obtained for the composition Co0.97Pd0.03Sb3 and reaches 4.3mWm−1K−2 at 700K. An activation energy, which can correspond to the intrinsic gap εG=0.13eV, is determined in Co0.98Ni0.02Sb3. Co1−xNixSb3 displays smaller electronic mobilities than in Co1−xPdxSb3 leading to smaller power factors. Best properties (3.4mWm−1K−2) are observed at 700K in Co0.95Ni0.05Sb3–Co0.94Ni0.06Sb3.
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