Interfacial Effect Boosts the Performance of All-Polymer Ionic Thermoelectric Supercapacitors

Ionic thermoelectric supercapacitors (ITESCs) have recently been developed for converting low-grade waste heat into electricity. Until now, most reports of ITESCs have been focused on the development of electrolytes, which then have been combined with a specific electrode material. Here, it is demonstrated that the electrode is not only critical for electrical energy storage but also greatly affects the effective thermopower (S-eff) of an ITESC. It is shown that the same ion gel can generate a positive thermopower in an ITESC when using gold nanowire (AuNW) electrodes, while generating a negative thermopower when using poly(3,4-ethylendioxythiophene):polystyrene sulfonate (PEDOT:PSS) electrodes. The achieved negative sign of the S-eff could be attributed to the Donnan exclusive effect from the polyanions in the PEDOT:PSS electrodes. After examining the thermovoltage, capacitance and charge retention performance of the two ITESCs, it is concluded that PEDOT:PSS is superior to AuNWs as electrodes. Moreover, a new strategy of constructing an ionic thermopile of multiple p- and n-type legs is achieved by series-connecting these legs with same electrolyte but different electrodes. Using interfacial effect at ionic gels/PEDOT:PSS electrode interface, an enhanced thermoelectric effect in ITESCs is obtained, which constitutes one more step towards efficient, low-cost, flexible, and printable ionic thermoelectric modules for energy harvesting.