Ultrahigh-Ionic-Conductivity, Antifreezing Poly(amidoxime)-Grafted Polyzwitterion Hydrogel for Facile Integrated into High-Performance Stretchable Flexible Supercapacitor

Developing wearable supercapacitors (SCs) with high stretchability, arbitrary deformability, and antifreezing ability is still a challenge. In the present work, an ultrahigh-ionic-conductivity, antifreezing poly(amidoxime)-graft-polyzwitterion (PAO-g-PSBMA) hydrogel electrolyte is fabricated by grafting PSBMA in PAO. Owing to the abundant hydrophilic and high ionic adsorption capacity of amidoxime groups in PAO and zwitterion groups in PSBMA, the as-prepared PAO-g-PSBMA hydrogel can facilitate the dissociation of lithium salt and exhibit an ultrahigh ionic conductivity of 29.8 S m^-1 at 25 °C and 3.4 S m^-1 even at -30 °C. Employing m_ATi₃C₂T_x and m_STi₃C₂T_x, which contain small amounts of PAO-AGE and PAO-g-PSBMA dispersions, respectively, coated onto both sides of the PAO-g-PSBMA hydrogel, we followed a thermal treatment to facilely form integrated stretchable flexible SCs. The as-prepared SCs show an outstanding recoverable tensile stain of 80% and an excellent electrochemical stability under many types and times of arbitrary deformation. More importantly, as-prepared m_ATi₃C₂T_x- and m_STi₃C₂T_x-based SCs present fantastic antifreezing ability and excellent stability with 74.6 and 78.3% retention of the initial capacitance, respectively, even after 1000 times of stretching to 60% at -30 °C. This work offers a new strategy of using PAO-grafted polyzwitterion for obtaining an antifreezing stretchable SC, which shows a high potential for application in next-generation integrated stretchable devices in various fields.