High-Conductivity and Ultrastretchable Self-Healing Hydrogels for Flexible Zinc-Ion Batteries

Aqueous zinc-ion batteries are promising candidates for flexible energy storage devices due to their safety, economic efficiency, and environmental friendliness. However, the uncontrollable dendrite growth and side reactions at the zinc anode hinder their commercial application. Herein, we designed and synthesized a dual network self-healing hydrogel electrolyte with zwitterionic groups (PAM–PAAS-QCS), which can be used for the large deformations of flexible devices due to its excellent stretchability (ε = 5100%). The incorporation of zwitterionic groups into the PAM–PAAS-QCS hydrogel electrolyte endows it with high ionic conductivity (33.61 mS/cm), a wide electrochemical stability window, and the ability to suppress zinc dendrite formation and side reactions. Besides, the Zn//Zn symmetric cell with PAM–PAAS-QCS can stably plate and strip zinc for 1500 h at 0.5 mA/cm2, and the Zn//Polyaniline full cell retains 82.4% of its capacity after 1500 cycles at 1 A/g. Additionally, flexible batteries based on both the original and self-healed PAM–PAAS-QCS hydrogel electrolytes demonstrate good cycling stability and stable charge–discharge performance under various bending conditions. This self-healing hydrogel electrolyte with excellent stretchability and high ionic conductivity is expected to pave the way for the development of high-performance flexible energy storage and wearable devices.