Snail Mucus-Inspired Interface: A Resilient and Self-Healing Double-Network Hydrogel Polymer Electrolyte for Flexible...

Flexible supercapacitors (SCs) have attracted considerable attention for wearable electronics, and developing high-performance electrolytes is critical for their practical application. While hydrogels have been widely investigated as solid electrolytes, studies on double-network (DN) hydrogel electrolytes specifically addressing the electrode-electrolyte interface stability under mechanical deformation remain relatively scarce. A major obstacle is maintaining a stable electrode-electrolyte interface under large mechanical deformation. Drawing inspiration from the mucus of a snail, which effectively adheres to various surfaces in challenging conditions, we present a self-healing xanthan gum/hydrophobically associated polyacrylamide/NaCl (XG/HPAAm/NaCl) hydrogel polymer electrolyte (HPE) that facilitates the creation of flexible SCs with improved mechanical and electrochemical properties. The optimized 2 wt% XG/HPAAm/0.4 M NaCl DN HPE exhibits a high ionic conductivity of 4.0 S/m, a tensile strength of 0.43 MPa, and an elongation at break of 11.7 mm/mm, along with a high adhesive energy of 254.7 J/m². The tough HPE was coated with a mixed adhesive of 502 cyanoacrylate glue and triethyl citrate (TEC) to create a surface coating resembling "mucus", onto which activated carbon (AC)-modified carbon cloth (CC) electrodes (CC/AC) were affixed on both sides to construct the flexible SCs. Investigations into the HPE's characteristics and the SCs' electrochemical performance at various bending angles reveal that the "mucus-coating" HPE exhibits strong electrode adhesion and significantly improved electrochemical performance. The assembled flexible SC delivers a high specific capacitance of 249.3 F/g at 0.30 A/g, retains 73.4% of its initial capacitance after 20,000 cycles, and maintains 86.9% capacitance retention under 180° bending, outperforming SCs assembled with original HPEs in both performance and stability. This approach provides a versatile method for improving the interfacial properties between electrodes and HPEs, paving the way for innovative applications in robust, self-healing, and flexible devices.