Recyclable, Self‐Healing Solid Polymer Electrolytes by Soy Protein‐Based Dynamic Network

Compared to traditional organic liquid electrolytes, which often present leakage, flammability, and chemical stability problems, solid polymer electrolytes (SPEs) are widely regarded as one of the most promising candidates for the development of safer lithium‐ion batteries. Vitrimers are a new class of polymer materials consisting of dynamic covalent networks that can change their topology by thermally activated bond‐exchange reactions. Herein, the recyclable and self‐healing solid polymer electrolytes (SPEs) with a soy protein isolate (SPI)‐based imine bond dynamic network are reported. This malleable covalent cross‐linked network polymer can be reshaped and recycled at high temperature (100 °C) or only with water at ambient temperature (25 °C), which may realize the green processing of energy materials. The introduction of bis(trifluoromethane) sulfonimide lithium (LiTFSI) significantly reinforces the conductivity of the dynamic network to a maximum of 3.3 × 10−4 S cm‐1. This simple and applicable method establishes new principles for designing scalable and flexible strategies for fabricating polymer electrolytes. The recyclable and self‐healing solid polymer electrolytes (SPEs) with a soy protein isolate (SPI)‐based imine bond dynamic network display favorable mechanical strength (77.4 MPa), high ionic conductivity (3.3 × 10−4 S cm−1). Thus, the SPEs based on the imine bond dynamic network of SPI is a promising platform for recyclable and repairable electrolytes.