Chemically Recyclable Pseudo-Polysaccharides from Living Ring-Opening Polymerization of Glucurono-1,6-lactones

Recent advances in synthetic methods and monomer design have given access to precision carbohydrate polymers that extend beyond native polysaccharides. In this article, we present the synthesis of a class of chemically recyclable ester-linked pseudo-polysaccharides via the living anionic ring-opening polymerization of glucurono-1,6-lactones. Notably, the pseudo-polysaccharides exhibited defined chain-end groups, well-controlled molecular weights, and narrow molecular weight distributions, all hallmarks of living polymerization. Furthermore, we demonstrate that our approach is modular, as evidenced by tunable glass transition temperatures (T_g) and the ability to produce both amorphous and semicrystalline polymers by adjusting the monomer side chain structure. Lastly, we showcased the complete catalytic chemical recycling of these pseudo-polysaccharides back to the monomers. The flexibility of the polymerization and the recyclability of these pseudo-polysaccharides promote a sustainable circular economy while offering the potential to access polysaccharide-like materials with tunable thermal and mechanical properties.