A self-healing anhydrous ionogel with high ionic conductivity enabled by dynamic network design for zinc metal batteries

Traditional gel electrolytes have hindered the practical application of zinc metal batteries due to their insufficient mechanical strength, poor self-healing capabilities, and substantial reliance on petroleum-based polymers. Here, we develop a self-healing ionogel electrolyte through a one-step, solvent-free synthesis, employing α-lipoic acid (LA) and hydroxypropyl cellulose (HPC) as a bio-based polymer framework. The ionogel features a three-dimensional (3D) dynamic network structure, constructed from the synergistic integration of reversible disulfide bonds, hydrogen bonds, and zinc-carboxylate coordination bonds. This dynamic network structure endows the ionogel with excellent self-healing properties, enabling rapid restoration of structural integrity and electrochemical performance after mechanical damage. Benefiting from continuous ion transport channels formed by nanoscale ionic clusters, this ionogel achieves a high ionic conductivity of 29.2 mS cm -1 , significantly promoting Zn 2+ migration. Furthermore, its electrochemical stability window is broadened to 2.39 V, surpassing that of traditional glass fiber (GF) separators. Consequently, zinc metal batteries assembled with this ionogel electrolyte demonstrate exceptional cycling stability, achieving stable cycling for over 1400 h at a current density of 0.5 mA cm -2 , with an average Coulombic efficiency (CE) of 99.6%. This work offers a promising and environmentally benign design toward highly stable and long-lasting zinc metal batteries.