Olefin Metathesis–Based Chemically Recyclable Polymers Enabled by a Fused-Ring Monomer

Abstract A promising solution to address the challenges in plastics sustainability is to replace current polymers with chemically recyclable ones that can depolymerise into their constituent monomers for circular use of materials. Despite the progress, few depolymerisable polymers exhibit the excellent thermal stability and strong mechanical properties of traditional polymers. Here we report a series of chemically recyclable polymers that show excellent thermal stability (decomposition temperature > 370 ºC) and tunable mechanical properties. The polymers are formed via ring-opening metathesis polymerisation of cyclooctene with a trans-cyclobutane installed at the 5,6-positions. The additional ring converts the non-depolymerisable polycyclooctene into a depolymerisable polymer by reducing the ring strain energy in the monomer (from 8.2 kcal/mol in unsubstituted cyclooctene to 4.9 kcal/mol in the fused ring). The fused-ring monomer enables a broad scope of functionalities to be incorporated, providing access to chemically recyclable elastomers and plastics that show promise as next-generation sustainable materials.