A Novel PDMS-Based Flexible Thermoelectric Generator Fabricated by Ag2Se and PEDOT:PSS/Multi-Walled Carbon Nanotubes with High Output Performance Optimized by Embedded Eutectic Gallium–Indium Electrodes

Flexible thermoelectric generators (FTEGs), which can overcome the energy supply limitations of wearable devices, have received considerable attention. However, the use of toxic Te-based materials and fracture-prone electrodes constrains the application of FTEGs. In this study, a novel Ag2Se and Poly (3,4-ethylene dioxythiophene): poly (styrene sulfonate) (PEDOT:PSS)/multi-walled carbon nanotube (MWCNT) FTEG with a high output performance and good flexibility is developed. The thermoelectric columns formulated in the work are environmentally friendly and reliable. The key enabler of this work is the use of embedded EGaIn electrodes, which increase the temperature difference collected by the thermoelectric column, thereby improving the FTEG output performance. Additionally, the embedded EGaIn electrodes could be directly printed on polydimethylsiloxane (PDMS) molds without wax paper, which simplifies the preparation process of FTEGs and enhances the fabrication efficiency. The FTEG with embedded electrodes exhibits the highest output power density of 25.83 μW/cm2 and the highest output power of 10.95 μW at ΔT = 15 K. The latter is 31.6% higher than that of silver-based FTEGs and 2.5% higher than that of covered EGaIn-based FTEGs. Moreover, the prepared FTEG has an excellent flexibility (>1500 bends) and output power stability (>30 days). At high humidity and high temperature, the prepared FTEG maintains good performance. These results demonstrate that the prepared FTEGs can be used as a stable and environmentally friendly energy supply for wearable devices.