Highly Deformable, Conductive Double-Network Hydrogel Electrolytes for Durable and Flexible Supercapacitors

Developing flexible energy storage devices with the ability to retain capacitance under extreme deformation is promising but remains challenging. Here, we report the development of a durable supercapacitor with remarkable capacitance retention under mechanical deformation by utilizing a physical double-network (DN) hydrogel as an electrolyte. The first network is hydrophobically associating polyacrylamide cross-linked by nanoparticles, and the second network is Zn2+ cross-linked alginate. Through soaking such a DN hydrogel into a high concentration of ZnSO4 solution, a highly deformable electrolyte with good conductivity is fabricated, which also shows adhesion to diverse surfaces. Directly attaching the hydrogel electrolyte to two pieces of an active carbon cloth facilely produces a flexible supercapacitor with a high specific capacitance and theoretical energy density. Remarkable capacitance retention under tension, compression, and bending is observed for the supercapacitor, which can also maintain above 87% of the initial capacitance after 4000 charge–discharge cycles. This study provides a simple way to fabricate hydrogel electrolytes for deformable yet durable supercapacitors, which is expected to inspire the development of next-generation flexible energy storage devices.