Unveiling Brass-Doped CoSb<sub>3</sub>-Based Thermoelectric Materials Using Solid-State Reaction.

Abstract

Skutterudite (CoSb₃)-based thermoelectric materials are regarded as one of the most promising candidates for mid-temperature commercial thermoelectric applications, thanks to their excellent electrical performance and alloy-based attributes. By utilizing techniques such as doping, microstructure design, and high-temperature solid-state reactions, synthesis of Brass_x/Co₄Sb_11.5Te_0.5 (x = 0.1, 0.3, 0.5, 0.7, representing wt%) in composite form can be rapidly achieved. XRD analysis indicates that the prepared Brass_x/Co₄Sb_11.5Te_0.5 samples primarily exhibit the CoSb₃ crystal structure, with the formation of minor impurity phases such as Cu₁₃Te₇ and ZnTe. SEM and EDS analyses reveal that the sample is composed of nanoscale equiaxed grains, some of which are micrometer in size, with a large number of microporous structures distributed uniformly, forming abundant grain boundaries. By co-doping with brass and tellurium (Te), the carrier concentration can be effectively regulated, thereby enhancing the power factor of CoSb₃-based thermoelectric materials. Meanwhile, the introduction of nanostructures, grain boundaries, and defects optimizes the microstructure of the samples, leading to a reduction in the lattice thermal conductivity of the CoSb₃-based thermoelectric materials. At a testing temperature of 781 K, Brass_0.1/Co₄Sb_11.5Te_0.5 achieved a maximum power factor of 1.86 mW·m^-1·K^-2, a minimum lattice thermal conductivity of 1.02 W/(mK), and a maximum thermoelectric figure of merit <i>ZT</i> of 0.81.