Abundant Hydrogen Bonds Formed in a Urea‐Based Gel Polymer Electrolyte Improve Interfacial Stability in Lithium Metal Batteries

As an emerging and potential replacement system for liquid electrolytes, polymer electrolytes (PEs) exhibit unique capacity in suppressing metal dendrite formation and leakage risks. However, the most used polymer matrix, including polyether, polyester, and polysiloxane, still cannot meet the practical demands for metal electrode compatibility and long lifespan. In this study, gel polymer electrolytes consisting of a polyurea network with abundant hydrogen bonds and deep eutectic electrolyte (DEE) are designed and prepared in-situ. The hydrogen bonding between polyurea chains and polyurea-DEE provides good interfacial stability between PEs and lithium metal. As a result, the assembled Li/LiFePO