A Light‐Mediated, 3D‐Printable, and Self‐Healable Polymer Electrolyte for Lithium Batteries

Abstract Self‐healing materials solutions and rapid prototyping approaches are actively searched to improve the safety and the production processes of batteries at the gigascale. Here, a self‐reparable polymer electrolyte designed into 3D‐printable ink formulation for digital light processing is shown. For this purpose, covalent adaptable networks containing hindered urea dynamic bonds end‐capped with photopolymerizable methacrylate groups are designed and investigated in terms of dynamicity and self‐healing properties. Electrochemical performance of the electrolytes is tested and compared with a commercially available benchmark, showing in all cases superior electrolyte uptake, ionic conductivities, and full specific capacity recovery after being cut in operando. This work brings the first self‐healable and 3D‐photoprinted electrolyte system for lithium batteries, at once ensuring safety, performance, and upscalability; the concept is also exploitable in lithium‐mediated ammonia electrosynthesis.