Wholly sustainable graft copolymers derived from cellulose, lignin, and hemicellulose for high-performance...

Sustainable elastomers derived from renewable biobased resources with excellent mechanical properties and varied functions are highly pursued to substitute traditional petroleum-based polymers yet challenging due to their limited macroscopic performance. In this work, we designed a series of wholly biobased cellulose-graft-poly(vanillin acrylate-co-tetrahydrofurfuryl acrylate) (Cell-g-P(VA-co-THFA) copolymer elastomers with cellulose as the rigid backbone, sustainable VA derived from lignin and soft THFA derived from hemicellulose as the hard and soft segments in the rubbery side chains. Moreover, the grafted side chains can be cross-linked to introduce an additional dynamic network structure via Schiff-base chemistry between the aldehyde and amino groups. The mechanical properties of Cell-g-P(VA-co-THFA) copolymer elastomers, including tensile strength, extensibility, elasticity, and toughness can be facilely manipulated by the VA/THFA feed ratio, cellulose content, and cross-linking density. These Cell-g-P(VA-co-THFA) copolymer elastomers are thermally stable and possess outstanding adhesion behavior and prominent UV-shielding performance. Besides dramatically enhanced mechanical properties, the cross-linked Cell-g-P(VA-co-THFA) counterparts exhibit remarkable shape memory behavior. This work provides a robust and convenient strategy for developing strong and versatile sustainable elastomers with different application demands by integrating different biomass feedstocks via elaborate molecular design.