Air-Assisted Sprayed Flexible Cellulose Acetate/Chitosan Materials for Food Packaging

Cellulose and chitin are the most abundant natural polymers, and their exploitation paves the way for sustainable materials and products. This work investigates the preparation of composites based on acetylated cellulose and partially deacetylated chitin, i.e., chitosan, using versatile and robust air-assisted solution spraying (AASS), a potential method for preparing materials both in situ and ex situ. These materials, in the form of films, despite being prepared from high-molecular-weight and rigid biopolymers, show high flexibility (Young's moduli below 1 GPa), outstanding mechanical properties (tensile strengths above 19 MPa and strain at failure higher than 2%), and bioactivity towards <i>E. coli</i>. The unprecedented flexibility, obtained without the use of any plasticizer or by casting with humidity control, is a direct consequence of the specific film morphology, whereby films are constituted from merging droplets. Depending on the solution properties (viscosity, surface tension), various droplet sizes are obtained, thus influencing the roughness and indirectly the wettability. Wettability analysis towards water and oil revealed higher contact angles towards both fluids as the content of chitosan increases in the composite what directly impacts packaging applications by better protecting the food. Besides this, higher chitosan content in the composite (7.5% <i>w</i>/<i>w</i>) enabled bioactivity against <i>E. coli</i>, where colony development was inhibited on the film surface compared with the neat cellulose acetate. This study shows a very high potential for AASS for obtaining uniform thin flexible films for food packaging applications, allowing faster drying and lower energy consumption than other film-forming techniques.