Super-stretching and high-performance ionic thermoelectric hydrogels based on carboxylated bacterial cellulose...

Self-powered sensors that do not require external power sources are crucial for next-generation wearable electronics. As environment-friendly ionic thermoelectric hydrogels can continuously convert the low-grade heat of human skin into electricity, they can be used in intelligent human-computer interaction applications. However, their low thermoelectric output power, cycling stability, and sensitivity limit their practical applications. This paper reports a 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-oxidized carboxylated bacterial cellulose (TOBC) coordination double-network ionic thermoelectric hydrogel with lithium bis(trifluoromethane) sulfonimide (LiTFSI) as an ion provider for thermodiffusion, as LiTFSI exhibits excellent thermoelectric properties with a maximum power output of up to 538 nW at a temperature difference of 20 K. The interactions between the ions and the hydrogel matrix promote the selective transport of conducting ionic ions, producing a high Seebeck coefficient of 11.53 mV K^-1. Hydrogen bonding within the polyacrylamide (PAAm) network and interactions within the borate ester bond within the TOBC confer excellent mechanical properties to the hydrogel such that the stress value at a tensile deformation of 3100 % is reaches 0.85 MPa. The combination of the high ionic thermovoltage and excellent mechanical properties ionic thermoelectric hydrogels provides an effective solution for the design and application of self-powered sensors based on hydrogels.