Gigantic and Continuous Output Power in Ionic Thermo‐Electrochemical Cells by Using Electrodes with Redox Couples

Abstract The main obstacle of ionic thermo‐electrochemical cells (TECs) in continuous power supply lies in a low heat‐to‐electricity energy conversion efficiency because most TECs work in thermodiffusion mode in which the ions are confined in a liquid/electrolyte media. The introduction of the redox couple onto the electrode surface may overcome the obstacle by resolving the low mass transport rate of ions caused by the redox process occurring near but not on the electrode surface. Herein, the authors demonstrate enhancement of TECs by integrating the redox couple directly onto the electrode surface to maximize the mass transport efficiency. A discontinuous interfacial modification strategy is developed by using a carbon cloth/iron (II/III) phytate as the symmetric electrodes. The gelled electrolyte consisting of a polyacrylamide matrix and phytic acid is shown to promote selective ion diffusion. A synergistic combination consisting of the thermodiffusion effect and redox reactions on the electrode is established in a pre‐treated layout. Such TEC affords a high output voltage of 0.4 V, an excellent instantaneous output power density (20.26 mW m^‐2 K^‐2) and a record‐high 2 h output energy density (2451 J m^‐2) under T_H = 30 °C with T_C = 15 °C, with an ultrahigh Carnot‐relative efficiency of 1.12%.