Polymer-to-Monomers Chemically Recyclable Poly(imide-imine) Plastics with Extreme-Condition Resistance and Flame Retardancy

Polyimides are a family of high-tech plastics that have irreplaceable applications in the fields of aerospace, defense, and opto-electronics, but polyimides are difficult to be reprocessed and recycled at the end of their service life, resulting in a significant waste of resources. Hence, it is of great significance to develop recyclable polyimides with comparable properties to the commercial products. Herein, we report a novel polymer-to-monomers chemically recyclable poly(imide-imine) (PtM-CR-PII) plastic, synthesized by cross-linking the amine-terminated aromatic bisimide monomer and the hexa-vanillin terminated cyclophosphazene monomer via dynamic imine bonds. The PtM-CR-PII plastic exhibits comparable mechanical and thermal properties as well as chemical stability to the commercial polyimides. The PtM-CR-PII plastic possesses a high Young’s modulus of ≈3.2 GPa and a tensile strength as high as ≈108 MPa, which also exhibits high thermal stability with a glass transition temperature of ≈220 °C. Moreover, the PtM-CR-PII plastic exhibits outstanding waterproofness, acid/alkali-resistance, and solvent-resistance, its appearance and mechanical properties can be well maintained after long-term soaking in water, highly concentrated acid and base, and various organic solvents. Furthermore, the cyclophosphazene moieties endow the PtM-CR-PII plastic with excellent flame retardancy. The PtM-CR-PII plastic exhibits the highest UL-94 flame-retarding rating of V-0 and a limiting oxygen index (LOI) value of 45.5%. Importantly, the PtM-CR-PII plastic can be depolymerized in an organic solvents-acid mixture medium at room temperature, allowing easy separation and recovery of both monomers in high purity. The recovered pure monomers can be used to regenerate new PtM-CR-PII plastics, enabling sustainable polymer-monomers-polymer circulation.