Phase transition driven tough hydrogel ionic thermoelectric cell with giant thermopower

The application of quasi-solid ionic thermoelectric (i-TE) cells holds great potential for powering ubiquitous wearable electronics without the need for cables or batteries. However, their practical application is restricted by low thermopower. Herein, a temperature-responsive supramolecular hydrogel, P(N-acryloylsemicarbazide-co-acrylic acid) (PNA), has been developed as a i-TE cell that integrates good mechanical and electrochemical properties. The volume phase transition (VPT) of PNA i-TE cell can generate a substantial ion entropy difference, thereby enhancing both the redox reaction efficiency and ionic thermodiffusion rate. A single PNA i-TE cell can generate a thermopower of 2.04 volts with a temperature difference of 50 K. The Seebeck coefficient (Se), specific output power density ( $${P}_{\max }/{(\Delta T)}^{2}$$ ) and figure of merit (ZT) of PNA i-TE cell can reach up to 40.9 mV K−1, 35.2 mW m−2 K−2 and 1.33 respectively. This ionic hydrogel is promising for the design of high performance polymer based i-TE cells in an environmentally friendly and cost-effective manner. Quasi-solid ionic thermoelectric cells are promising for wearable electronics, though it is challenging to fabricate devices due to low thermopower. Here the authors report a supramolecular hydrogel to enhance the thermopower for wearable electronics.