Healable and Reprocessable PETG-Based Dynamic Vinylogous Urethane Networks

The growing demand for sustainable materials calls for innovative strategies to extend the lifetime of polymers. In response to this challenge, we explored healable and reprocessable vinylogous urethane (VU) networks derived from commercially available glycol-modified polyethylene terephthalate (PETG). These materials were synthesized via Zn-catalyzed transesterification of PETG with ethylene glycol, end-functionalization of the resulting telechelics with bis-acetoacetate, and subsequent VU network formation using tris-(2-aminoethyl)-amine (TREN). The resulting networks combine high tensile strength (up to 48 MPa), high stiffness (0.9 GPa), and appreciable ductility (elongation at break up to 7%). An optimized network composition was reprocessed multiple times with minimal loss in performance and exhibits highly efficient healing behavior, recovering 95% of its original strength after 15 min at 180 °C. Overall, this work presents a simple and scalable route to transform a commercial high-performance polyester into a reprocessable and healable material that offers extended lifetime and improved sustainability.