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Self-healing and thermo bonding nanocellulose-vitrimer films

Naghmeh Nasiri (Monash University), David Joram Mendoza (Monash University, De La Salle University), Joel F. Hooper (Monash University), Warren Jeffrey Batchelor (Monash University), Matthieu Grésil (Monash University), Gil Garnier (Monash University)

Advanced Composites and Hybrid Materials
DOI: 10.1007/s42114-026-01840-5 (Materials Science)
Licence : CC BY

Résumé : Abstract This study demonstrates the scalable fabrication of novel cellulose nanocrystal (CNC)-vitrimer composite films through a simple dip-coating process followed by in situ polymerization. FTIR analyses confirm rapid monomer uptake and complete vitrimer network formation within 8 h at 145 °C, evidenced by the disappearance of epoxide and carboxyl peaks and the emergence of ester linkages. XPS and diffusion-edited 1 H NMR provide evidence consistent with covalent attachment of vitrimer species to the CNC surface, supporting the formation of a chemically integrated hybrid interface. Cross-sectional SEM imaging uncovers a stratified architecture comprising vitrimer-rich surface layers, an unmodified CNC core, and a chemically fused transition zone that promotes strong interfacial adhesion. Rheological and stress-relaxation measurements confirm vitrimeric behaviour with a low activation energy of 38.8 kJ/mol and a topology freezing temperature of 40 °C, enabling thermally triggered network rearrangement. Incorporation of the vitrimer phase substantially enhances mechanical performance, increasing elongation at break from 1.5% to 4.4% and toughness from 41 to 76 kJ/m³. Vitrimer integration also significantly improves humidity resilience, at 50% RH, water-vapor permeability decreases to 2.4 × 10⁻¹² g/Pa·s·m, and at elevated RH the composite film maintains nearly an order-of-magnitude lower permeability than the control CNC film. In addition, the vitrimer layer introduces multifunctional capabilities, including thermally activated healing, heat-sealability at 180 °C via dynamic bond exchange, and UV-shielding properties. This study presents a novel general and scalable strategy for chemically integrating dynamic vitrimer networks with nanocellulose. It provides a new material design to overcome humidity sensitivity for multifunctional sustainable bio-based films.

Publié le 09 Mai. 2026