To fulfill the ever-increasing power demands of deep space exploration, the output performance of radioisotope thermoelectric generators, the only accessible power source, must be enhanced in several aspects, including thermoelectric properties of materials, geometry, welding, etc. In this study, we present our results on the development of a novel thermoelectric slurry suitable for the 3D printing of thermoelectric generators with optimized leg geometry. The rheological properties of the slurry are optimized by combining proper amounts of organic solvent, binder, and bismuth telluride-based thermoelectric powder. The addition of Cu to the slurry as a conductive additive are also investigated. The homogeneous dispersion of Cu within the material not only increases the electrical conductivity of the final thermoelectric leg significantly but also promotes the crystallization of the thermoelectric particles during the sintering process. These effects result in 3D-printed thermoelectric composites exhibiting ZT values up to 0.91 and extended optimum operating temperature range. Thermoelectric modules composed of 3D-printed thermoelectric legs show excellent output performance and structural strength. This work could also produce other special shaped thermoelectric devices to match irregularly shaped heat sources to reduce contact heat loss and improve output performance.
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