Enhanced Output Performance of All-Solution-Processed Organic Thermoelectrics: Spray Printing and Interface Engineering

We report two organocompatible strategies to enhance the output performance of all-solution-processed poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) thermoelectric generators (TEGs): introducing an additive spray printing process and functionalized polymer interlayers to reduce the module resistance. The spray printing enabled the deposition of 1-μm-thick PEDOT:PSS layers with a high degree of design freedom, resulting in a significantly reduced sheet resistance of 16 Ω sq–1 that is closely related to the thermoelectric output performance. Also, by inserting an ultrathin silane-terminated polystyrene (PS) interlayer between the PEDOT:PSS thermoelectric layers and inkjet-printed Ag interconnects selectively, the contact resistivity extracted by the transmission line method was reduced from 6.02 × 10–2 to 2.77 × 10–2 Ω cm2. We found that the PS interlayers behaved as a thin tunneling layer, which facilitated the carrier injection from the inkjet-printed Ag electrodes into the PEDOT:PSS films by field emission with an effectively lowered energy barrier. The activation energy was also extracted using the Richardson equation, resulting in a reduction of 2.59 ± 0.04 meV after the PS treatment. Scalable plastic-compatible processability and selective interface engineering enabled to demonstrate the flexible 74-leg PEDOT:PSS TEGs exhibiting the open-circuit voltage of 9.21 mV and the output power of 2.23 nW at a temperature difference of 10 K.