Effect of Environment on Acetylated Cellulose Nanocrystal-Reinforced Biopolymers Films

Cellulose nanocrystals (CNCs) were acetylated to the various parametrised degrees of substitution (DS), determined through attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and incorporated into alginate (ALG) and chitosan (CH) film-forming solutions. An investigation of morphology with scanning electron microscopy (SEM) revealed increased chemical compatibility with the CH matrix after acetylation, producing a smooth surface layer, while ALG mixed better with pristine CNCs. The ATR-FTIR analysis of films demonstrated inter-diffusional structural changes upon the integration of pristine/modified CNCs. Films were evaluated in terms of water contact angle (WCA), which decreased upon CNC addition in either of the biocomposite types. The H₂O barrier assessed through applicative vapour transmission (WVT) rate increased with the CNC esterification in CH, but was not influenced in ALG. To evaluate the relationship between environmental humidity and mechanical properties, conditioning was applied for 48 h under controlled relative humidity (33%, 54% and 75%) prior to the evaluation of the mechanical properties and moisture content. It was observed that tensile strength was highest upon specimens being dry (25 ± 3 MPa for ALG, reinforced with neat CNCs, or 16 ± 2 MPa in the CH with CNCs, reacting to the highest DS), lowering with dewing, and the elongation at break exhibited the opposite. It is worth noting that the modification of CNCs improved the best base benchmark stress-strain performance. Lastly, (thermal) stability was assessed by means of the thermogravimetric analysis (TGA) technique, suggesting a slight improvement.