A light-mediated, 3D-printable, and self-healable polymer electrolyte for lithium batteries

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.