Self‐Healing Polymer Electrolytes Formed via Dual‐Networks: A New Strategy for Flexible Lithium Metal Batteries

Abstract A novel polymer electrolyte with mechanically robust and self‐healing properties was fabricated through a dual‐network structure, crosslinked by quadruple hydrogen bonding and chemical bonding. The dynamic ureido‐pyrimidinone (UPy) dimers were the first network in the polymer matrix. This group endows the polymer electrolyte with good self‐healing capacity and improves the reliability and lifetime of the polymer lithium batteries. The crosslinked polyethylene glycol‐bis‐carbamate dimethacrylate (PEGBCDMA) is the second network and guarantees dimensional stability and good mechanical properties of the polymer electrolyte. The dual‐network self‐healing polymer electrolyte (DN‐SHPE) exhibits improved ionic conductivity versus the polymer electrolyte fabricated by poly(ethylene glycol) diacrylate (PEGDA). It has high thermal stability (up to 350 °C) and excellent interfacial stability with the electrodes. When the DN‐SHPE‐based cells were fabricated with LiFePO 4 and Li metal, the resulting cells show good reversible specific capacity and considerable rate capability. Moreover, the pouch cell could maintain electrochemical function even under deformation or folding conditions.