Fabrication, spark plasma consolidation, and thermoelectric evaluation of nanostructured CoSb3

•Fabrication of nanostructured thermoelectric skutterudite in large scale.•Maintaining nanostructure using spark plasma sintering (SPS).•Demonstrate dramatically reduced thermal conductivity due to nanostructuring.•Significantly improved figure of merit as compared to pure compound.•Demonstrate TE performance stability over time. Nanostructured powders of thermoelectric (TE) CoSb3 compounds were synthesized using a chemical alloying method. This method involved co-precipitation of oxalate precursors in aqueous solution with controlled pH, followed by thermochemical treatments including calcination and reduction to produce stoichiometric nanostructured CoSb3. Moreover, CoSb3 nanoparticles were consolidated by spark plasma sintering (SPS) with a very brief processing time. Very high compaction densities (>95%) were achieved and the grain growth was almost negligible during consolidation. An iterative procedure was developed to maintain pre-consolidation particle size and to compensate Sb evaporation during reduction. Significant changes in particle size and morphology were observed, and the post-reduction cooling was found to be an important stage in the process. The spark plasma sintering (SPS) parameters were optimized to minimize the grain growth while achieving sufficient densification. Grain sizes in the range of 500nm to 1μm, with compaction density of 95–98% were obtained. Preliminary measurements of thermal diffusivity and conductivity showed the dependence on grain size as well as on porosity. TE transport properties were measured in the temperature range of 300–650K. Sample showed p-type behavior with a positive Seebeck coefficient, which increases with increasing temperature. Electrical conductivity measurements indicate metallic behavior and it decreases with increasing temperature. Thermal conductivity also decreases with increasing temperature and major contribution is due to the lattice component. A TE figure of merit of 0.15 was achieved for high purity CoSb3 nanostructured TE material at 650K and these results are comparable with the values reported for the best unfilled/undoped CoSb3 in the literature.