High-Performance Biobased Elastomers with Both High Strength and High Toughness

Harvesting sustainable biobased elastomers with both high strength and high toughness holds great promise for various applications. However, the inherent conflicts between these properties make it challenging to achieve a simultaneous balance. Here, inspired by the structure of spider silk, we have synthesized a multiphase polymer (PA-BPx) containing oxalamides derived from biomass. The introduction of a benzene ring structure, combined with the double hydrogen bonds of oxalamide, results in smaller and more uniformly distributed hard domains, concurrently enhancing the molecular chain rigidity. The molecular structure described facilitates energy dissipation through the destruction and reformation of hard domains, achieving a remarkable balance between superior mechanical robustness and toughness. The PA-BP40 elastomer demonstrates exceptional advantages in both tensile strength and toughness compared to other reported biobased and filled biobased elastomers, with a toughness of 230 MJ·m–3 and maintaining a high tensile strength of 46.6 MPa. These remarkable mechanical properties make the PA-BP40 elastomer a promising material for various applications where both high strength and toughness are required. Moreover, the elastomers exhibit strong fluorescence even in the absence of conventional chromophores, highlighting their potential for fluorescent anticounterfeiting applications. Overall, this study presents a promising strategy for developing sustainable elastomers with desirable performance characteristics, thus contributing to the advancement of biobased materials in various applications.