Rediscovering Surlyn: A Supramolecular Thermoset Capable of Healing and Recycling

Surlyn consists of ionomers of poly(ethylene-co-methacrylic acid) (PEMA) partially neutralized with metal ions. Considering its huge consumption every year, it is highly desirable to realize efficient healing and recycling of Surlyn through an easily available method. Herein, healable and recyclable Surlyn materials are fabricated by complexation of PEMA with Zn²⁺ ions followed by a hot-pressing process. The PEMA/Zn composites exhibit a tensile strength of ≈37 MPa, Young's modulus of ≈343 MPa, and toughness of ≈95 MJ m^-3 . Structural analysis discloses that the PEMA/Zn composites are dynamically cross-linked with coordination interactions and reinforced with polyethylene nanocrystals, and have the typical structure of supramolecular thermosets. As supramolecular thermosets, the reversibility of coordination interactions endows the PEMA/Zn composites with good healing and recycling capacities. The PEMA/Zn composites can fully heal mechanical damage to restore their original mechanical strength when heated at 90 °C. Under a pressure of 3 MPa at 100 °C, the PEMA/Zn composites can be recycled multiple times to regain their structural integrity and mechanical properties.