• Cellulose nanocrystals used as cocross-linkers in bionanocomposite hydrogels.
  • β-alanine maleimide successfully used for cellulose nanocrystal functionalization.
  • Diels-Alder reaction with maleimide-capped nanocrystals led to more stable gels.
  • Swelling and viscoelastic properties influenced by grafted cellulose nanocrystals.

Abstract

This article deals with the preparation of bionanocomposite hydrogels from natural polymers and nanoentities, an emerging class of materials for biotechnological and biomedical applications. Herein, the applicability of the Diels-Alder “click” reaction to the design of bionanocomposite hydrogels from furan modified gelatin using maleimide-functionalized cellulose nanocrystals as multifunctional cocross-linkers is demonstrated. The functionalization of cellulose nanocrystals with maleimide moieties was confirmed by XPS. The swelling and rheological properties of the resulting bionanocomposite confirmed the formation of hydrogel networks with covalently embedded nanoentities. The Diels-Alder reaction resulted in the formation of stiffer networks with lower swelling ratios due to the formation of additional cross-linking points. The designed “click” strategy proved to be a promising candidate for the formation of fully renewable bionanocomposite hydrogels.