Hierarchical Assembly of Nanocellulose into Filaments by Flow-Assisted Alignment and Interfacial Complexation:...

Filaments comprising solely cellulose nanofibrils (CNFs) have been fabricated by flow-assisted assembling, where the strength can be improved greatly with the sacrifice of toughness. Inspired by the architecture of natural nacre and plant cell wall, the combined technique of convergent microfluidic spinning and in situ interfacial complexation between CNF and chitosan molecules was used to construct the filaments with hierarchical assembly of highly oriented CNFs locked by chitosan complexes, showing simultaneous enhancements of strength and toughness. In specific, the best performing filament exhibited a toughness of 88.9 kJ/m³ and a tensile strength of 1289 MPa because of the strong interfacial complexation interactions between CNFs and chitosan molecules. The tensile strength was further raised to 1627 MPa when the filaments were cross-linked synergistically by using Ca²⁺, surpassing the reported values in the literature. Molecular dynamics simulations revealed the possible fracture mechanism of the filaments under tension. With excellent mechanical performance and biocompatibility, the resulting CNF/chitosan filament system showed a promising application potential as nonabsorbable surgical sutures. The demonstrated spinning technology also offered a new avenue for the fabrication of high-performance filaments.