Stretchable and Self-Healing Integrated All-Gel-State Supercapacitors Enabled by a Notch-Insensitive Supramolecular Hydrogel Electrolyte

Next-generation wearable electronics are expected to endure significant deformations and mechanical damage. Therefore, self-healing stretchable electrolytes with high ionic conductivity and robust mechanical strength, which have high tolerance of deformations and spontaneously recover electrochemical properties after external damage, are necessary conditions for the realization of flexible supercapacitors. Here, a new type of zwitterionic supramolecular hydrogel cross-linked through rationally designed ionic associations and hydrogen bonds is reported (PAD/H2SO4). The resultant supramolecular network realizes a high ionic conductivity of 57 mS cm–1 and unprecedented mechanical properties such as a high toughness of 35 000 J m–2, a notch-insensitive of up to 2200% strain, and efficient instantaneous self-healing within 5 min. Acting as an electrolyte, a novel flexible supercapacitor design strategy is proposed by integrating capacitive materials directly onto the PAD/H2SO4 hydrogel to achieve exceptional electrochemical performance, which can be repeatable for at least 50 cutting/healing cycles. The facile and versatile strategy for the construction of the integrated all-gel-state supercapacitors with self-healing stretchable electrolytes will provide new directions for future long-life flexible devices.