The development of polymer products with a circular economy lifecycle represents a path to alleviate the growing plastic waste and energy crisis. However, long-standing challenges include synthesis scalability, tunable material performance and the feasibility of chemical recycling from mixed products. Here we developed a facile regioirregular polymerization strategy to access diverse polymer structures from a single monomer via regioselectivity and dynamic covalent bond exchange. We were able to synthesize polyurethanes (PU x , where x represents the percentage of urethane linkages in the polymer) with tailored urethane contents by modulating the reaction time for the regioirregular polymerization of tetramethylene urethane. The resulting PU x products showcase remarkable composition-dependent material performance, illustrating high strength, toughness and gas barriers comparable with commercial plastics. In particular, PU57 exhibits superior adhesive strength, outperforming commercial glues. Notably, these diverse PU x products could be converted back to a single monomer, representing a proof-of-concept process for a ‘single monomer ↔ multiple polymers’ closed loop.
Ha et al. (Thu,) studied this question.