Self-healing, deformable and safe integrated supercapacitor enabled by synergistic effect of multiple physical interactions in gel polymer electrolyte with dual-role Co2+

With the rapid development of wearable electronic devices, flexible supercapacitors have gained strong interest. However, traditional sandwich supercapacitors have weak interfacial binding, resulting in high interface resistance and poor deformability. Herein, a self-healing integrated supercapacitor based on a polyacrylic acid-polyisodecyl methacrylate-CoSO 4 gel polymer electrolyte (GPE) was developed. By incorporating ion coordination into a hydrophobic association network, a double network structure was formed, endowing the GPE with remarkable mechanical properties and self-healing abilities. Specifically, Co 2+ ions functioned both as charge carrier and crosslinker, simultaneously enhancing the electrochemical (2.87 S/m) and mechanical (0.262 MPa) properties of the GPE. In situ growth of polyaniline electrode material on the GPE surface resulted in an integrated supercapacitor with a continuous morphology at the electrode/electrolyte interface, minimizing interface resistance and improving electrochemical performance. The supercapacitor exhibits high specific capacitance, exceptional cyclic stability, superior deformability and security due to the unique integrated structure. Furthermore, it demonstrates remarkable electrochemical and self-healing properties even at quite low temperature. Overall, this work offers a promising approach for reliable self-healing energy storage devices with high performance and adaptability to complex usage conditions.