Closed-Loop Recycling of Mixed Plastics of Polyester and CO₂-Based Polycarbonate to a Single Monomer

Physical blending is an effective strategy for tailoring polymeric materials to specific application requirements. However, physically blended mixed plastics waste adds additional barriers in mechanical or chemical recycling. This difficulty arises from the intricate requirement for meticulous sorting and separation of the various polymers in the inherent incompatibility of mixed polymers during recycling. To overcome this impediment, this work furthers the emerging single-monomer - multiple-materials approach through the design of a bifunctional monomer that can not only orthogonally polymerize into two different types of polymers - specifically lactone-based polyester and CO₂-based polycarbonate - but the resultant polymers and their mixture can also be depolymerized back to the single, original monomer when facilitated by catalysis. Specifically, the lactone/epoxide hybrid bifunctional monomer (BiL^O) undergoes ring-opening polymerization through the lactone manifold to produce polyester, PE(BiL^O), and is also applied to ring-opening copolymerization with CO₂, via the epoxide manifold, to yield polycarbonate, PC(BiL^O). Remarkably, a one-pot recycling process of a BiL^O-derived PE/PC blend back to the constituent monomer BiL^O in >99 % selectivity was achieved with a superbase catalyst at 150 °C, thereby effectively obviating the requirement for sorting and separation typically required for recycling of mixed polymers.