Biobased, self-healable, high strength rubber with tunicate cellulose nanocrystals.

Cellulose nanocrystals represent a promising and environmentally friendly reinforcing nanofiller for polymers, especially for rubbers and elastomers. Here, a simple approach via latex mixing is used to fabricate biobased, healable rubber with high strength based on epoxidized natural rubber (ENR). Tunicate cellulose nanocrystals (t-CNs) isolated from marine biomass with a high aspect ratio are used to improve both mechanical properties and self-healing behavior of the material. By introducing dynamic hydrogen bond supramolecular networks between oxygenous groups of ENR and hydroxyl groups on the t-CN surface, together with chain interdiffusion in permanently but slightly cross-linked rubber, self-healing and mechanical properties are facilitated significantly in the resulting materials. Macroscopic tensile healing behavior and microscopic morphology analyses are carried out to evaluate the performance of the materials. Both t-CN content and healing time have significant influence on healing behavior. The results indicate that a synergistic effect between molecular interdiffusion and dynamic hydrogen bond supramolecular networks leads to the improved self-healing behavior.