High-Performance Biobased Polyesters with High Gas Barrier, Glass Transition Temperature, and Tensile Strength Enabled by Hydrogen Bonds and Flexible Segments

High-performance biobased polyesters with excellent thermal, mechanical, and gas barrier properties are in demand nowadays, while current design strategies have failed to endow polyesters with such integrated performances synchronously. Herein, we synthesize a series of furan-based copolyesters poly(butylene 4-hydroxy-N-(2-hydroxyethyl)2,5-furandicarboxylate) (PBAnF) containing an amide structure and flexible aliphatic segments in the main chains via condensed polymerization. The resultant copolyester PBA20F records balanced pre-eminent mechanical properties including tensile strength (78.0 MPa) and a large elongation at break (199%) while exhibiting a high glass transition temperature (54 °C) and a good enough gas barrier property. Such integrated excellent performances of copolyesters are ascribed to the combined effects of introduced intermolecular hydrogen bonds and flexible segments. Besides, PBAnFs still display high optical transparency in the visible region. This work provides an innovative design strategy to prepare a new class of advanced furan-based copolyesters with remarkable mechanical, thermal, and gas barrier properties, thus supplying a series of promising high-performance biobased copolyesters for potential packaging applications.