Extremely Tough, Stretchable Gel Electrolytes with Strong Interpolymer Hydrogen Bonding Prepared Using Concentrated Electrolytes to Stabilize Lithium‐Metal Anodes

Abstract Extremely tough and stretchable gel electrolytes, which can be prepared by leveraging the strong interpolymer hydrogen bonding in concentrated lithium (Li)‐salt electrolytes, are reported. These electrolytes can be realized by optimizing the competitive hydrogen‐bonding interactions between polymer chains, solvent molecules, Li cations, and counteranions. Free polar solvent molecules, which typically impede interpolymer hydrogen bonding, are scarce in concentrated electrolytes; this feature can be exploited to prepare hydrogen‐bonded gel electrolytes with unprecedented toughness. In contrast, free solvent molecules are abundant in electrolytes with typical concentrations, yielding considerably weaker gel electrolytes. The tough gel electrolyte can be used an artificial protective layer for Li‐metal anodes, as it considerably enhances the cycling stability of a Li symmetric cell through uniform Li deposition/dissolution. Additionally, employing the gel electrolyte as the protecting layer significantly improves the cycling performance of the Li||LiNi_0.6Co_0.2Mn_0.2O₂ full cell.