Healable Glassy Metallosupramolecular Polymers

Metallosupramolecular polymers (MSPs), formed through ligand-metal coordination, feature dynamic bonds that enable damage repair via reversible dissociation. Here, we report the synthesis of healable MSPs by modifying commercially available glycol-modified polyethylene terephthalate (PETG), an amorphous commodity polyester known for its durability, chemical resistance, and formability. The new materials were accessed through the Zn-catalyzed transesterification of PETG with ethylene glycol, end-functionalization of the resulting homobifunctional oligomers with the 2,6-bis(1'-methylbenzimidazolyl)pyridine (Mebip) ligand, and subsequent assembly of these macromonomers into MSPs via Zn²⁺ complexation. One of the MSPs made offers an attractive combination of high tensile strength (31 MPa), high Young's Modulus (1 GPa), and excellent healability (94% in 2.5 min).