Recyclability and Self‐Healing of Dynamic Cross‐Linked Polyimide with Mechanical/Electrical Damage

Recyclability and self‐healing are two most critical factors in developing sustainable polymers to deal with environmental pollution and resource waste. In this work, a dynamic cross‐linked polyimide insulation film with full closed‐loop recyclability is successfully prepared, which also possesses good self‐healing ability after being mechanical/electrical damaged depending on the Schiff base dynamic covalent bonds. The recycled and self‐healed polyimide film still maintain its good tensile strength ( σ t ) >60 MPa with Young's modulus ( E ) >4 GPa, high thermal stability with glass transition temperature ( T g ) >220 °C, and outstanding insulation property with breakdown strength ( E 0 ) >358 kV mm −1 , making it a very promising low energy consumption and high temperature resistant insulation material. The strategy of using Schiff base dynamic covalent bonds for reversible repairing the structure of high T g polyimides promotes the wider application of such sustainable and recyclable material in the field of electrical power and micro‐electronics.