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Traditional thermoelectric generators (TEGs) face scalability challenges due to high-temperature, long-duration curing processes and rare-earth/toxic chalcogenides such as bismuth telluride. 

In this study, we used n-chitosan-Bi2Te2.7Se0.3 and p-chitosan-Bi0.5Sb1.5Te3 composite inks to print a circular thermoelectric generator (TEG) device using a low-energy-input curing method. Thermoelectric (TE) composite films were fabricated using varying sizes of thermoelectric particles and a small chitosan binder (0.05 wt. %). The particles and binder were hot pressed at an applied pressure of 200 MPa and cured at 200 °C for 30 min. We achieved ZT of 0.35 for the n-type and 0.7 for the p-type TE composite films measured at room temperature. A radial TEG was fabricated using the best-performing n-type and p-type composite inks and achieved a power output of 87 µW and a power density of 727 µW/cm2 at a temperature difference of 35 K; these are among the best-reported values for printed TEG devices. Using a low-energy-input fabrication method, we eliminated the need for high-temperature and long-duration curing processes to fabricate printing devices. Thus, we envisage that the low-energy-input curing process and cost-effective printable strategy presented in this work pave the way for sustainable manufacturing of large-scale energy harvesting TEG devices. 

This work presents an energy efficient technique for fabricating flexible thermoelectric generators while using printable ink. We have fabricated thermoelectric composite thick films using two different mesh sizes of n-type bismuth particles, various binder to thermoelectric material weight ratios, and two different pressures, 200 MPa and 300 MPa, in order to optimize the thermoelectric properties of the composite films. The use of chitosan dissolved in dimethylsulfoxide with less than 0.2 wt. % of chitosan, the first time chitosan has been used in this process, was sufficient for fabricating TE inks and composite films. Low temperature curing processes, along with uniaxial pressure, were used to evaporate the solvent from the drop-casted inks. This combination reduced the temperature needed compared to traditional curing processes while simultaneously increasing the packing density of the film by removing the pores and voids in the chitosan-bismuth composite film. Microstructural analysis of the composite films reveals low amounts of voids and pores when pressed at sufficiently high pressures. The highest performing composite film was obtained with the weight ratio of 1:2000 binder to bismuth, 100-mesh particle size, and 300 MPa of pressure. The best performing bismuth chitosan composite film that was pressed at 300 MPa had a power factor of 4009 ± 391 μW/m K2 with high electrical conductivity of 7337 ± 522 S/cm. The measured thermal conductivity of this same sample was 4.4 ± 0.8 W/m K and the corresponding figure of merit was 0.27 at room temperature.