Self-Healing Solid Polymer Electrolyte with High Ion Conductivity and Super Stretchability for All-Solid Zinc-Ion Batteries

The zinc-ion battery (ZIB) is a novel energy storage device, an attractive alternative to the lithium-ion battery. The frequently used aqueous electrolyte suffers from many problems such as zinc dendrites and leakage, which prompts hydrogel electrolytes and solid electrolytes as good replacements. However, hydrogel electrolytes are usually unstable, owing to water volatilization. Herein, a novel solid polymer electrolyte (SPE) utilizing coordination of zinc ions is designed and then introduced into an all-solid ZIB. Benefiting from the unique coordination structure between the polymer and zinc ions, the SPE shows outstanding flexibility, high ion conductivity, and self-healing properties. In addition, the imine bonds in the polymer allow the electrolyte to degrade in acid environments, endowing its recyclability. More importantly, solid-state ZIBs based on the polymer electrolytes exhibit an impressive cycling stability (125% capacity retention after 300 cycles) and a high coulombic efficiency (94% after 300 cycles). The results demonstrate the promising potentials of the developed SPEs that can be used in all-solid ZIBs.