Highly Flexible and Foldable Paper-Based Thermoelectric Generator Prepared with Post-Treatment-Free PEDOT:PSS Hybrid Ink

Paper-based thermoelectric (PTE) generators have recently emerged as a green technology that can help alleviate environment pollution and the energy crisis. In this work, a PTE generator was prepared by coating a post-treatment-free thermoelectric ink consisting of poly(3,4-ethylenedioxythiophene)/polystyrene sulfonate (PEDOT:PSS) doped with 1-ethyl-3-methylimidazolium:tricyanomethanide (EMIM:TCM) onto the card paper. By tuning the molar concentration of the EMIM:TCM to 0.17 M and with hot-pressing, the PTE generator showed a decent power factor (PF) value of 6.82 μW m−1 K−2, which was higher than the values of PTE in the literature. This phenomenon could be attributed to the synergistic effect of high-performance thermoelectric ink (i.e., PF = 175 μW m−1 K−2 when deposited on glass slide) and the hot-pressing. The hot-pressing enhanced the packing density of cellulose fibers and the associated PEDOT:PSS hybrid, which enabled the formation of long-range conductive paths. In addition, the PTE had good mechanical stability, indicated by no significant change of the power factor values after cyclic folding 10,000 times. Moreover, the structure of as-prepared PTE could be easily tuned into different shapes that are promising for the preparation of flexible wearable thermoelectric generators.