Reinforcement of all-cellulose nanocomposite films using native cellulose nanofibrils

• All-cellulose nanocomposites were fabricated using CNFs as the reinforcement.
• CNFs greatly enhanced mechanical properties of the nanocomposite films.
• An optimal CNFs concentration of 10 wt% in the composites was found.
• The nanocomposite films exhibited excellent optical transparency.
• The nanocomposite films exhibited enhanced thermal stability.

All-cellulose nanocomposite films were prepared using native cellulose nanofibrils (CNFs) as fillers and lithium chloride/N,N-dimethylacetamide (LiCl/DMAc) dissolved regenerated cellulose as the matrix. The CNFs, with diameters in the range of 15–40 nm were obtained by combined physical methods of ultrasonic treatment and high shear homogenization. The morphology, structure, and properties of the nanocomposite films were characterized by scanning electron microscope (SEM), X-ray diffraction (XRD), optical transmittance, thermal gravimetric analysis (TGA), and mechanical testing. The nanocomposite films exhibited good optical transparency, thermal stability, and remarkably enhanced mechanical properties compared to the regenerated cellulose matrix. By varying the CNFs content, the tensile strength of the nanocomposite films increased from 61.56 MPa to 99.92 MPa and the Young's modulus increased from 0.76 GPa to 4.16 GPa. This work provided a promising pathway for manufacturing high performance and environmental-friendly all-cellulose nanocomposites.