High-performance, anti-freezing all-gel-state supercapacitor with full-device self-healing and extreme damage tolerance based on a redox-active zwitterionic organohydrogel

초록

In this study, we report an interface-engineered all-gel-state supercapacitor based on a multifunctional zwitterionic organohydrogel for durable wearable electronics. The device integrates a Fe3+/Fe(2+)redox-active organohydrogel electrolyte with CNT/PANI-based gel electrodes sharing an identical dynamic polymer network, together with an Au nanosheet current collector and a vitrimer-like polyurethane substrate. The shared dynamic polymer network enhances electrode-electrolyte interfacial compatibility and effectively stabilizes the interface under repeated deformation and damage. The Fe3+/Fe(2+)redox reactions provide additional Faradaic charge storage, enabling a high areal capacitance of 1418.3 mF cm(-2)at 0.5 mA cm(-2). In addition, zwitterionic betaine facilitates reversible electrostatic interactions within the dynamic network, enabling outstanding self-healing performance. The fully integrated supercapacitor recovers up to 95% of its initial capacitance after complete bisection and healing and retains similar to 85% after five damage/healing cycles. Strong hydrogen-bonding interactions among ethylene glycol, betaine, and water suppress freezing and dehydration, enabling stable operation over a wide temperature range from -30 to 50 degrees C. The device maintains over 80% of its initial capacitance after 10,000 charge-discharge cycles and exhibits robust electrochemical stability under bending, folding, and severe puncture damage. Furthermore, vertical integration of the supercapacitor with an organohydrogel-based strain sensor enables reliable motion monitoring even after repeated damage and healing. These results establish an interface-engineered all-gel-state energy-storage platform that simultaneously achieves high capacitance, interfacial stability, self-healing, mechanical robustness, and wide-temperature operation for next-generation wearable electronics.

키워드