Self-Assembly of Hierarchically Structured Cellulose@ZnO Composite in Solid–Liquid Homogeneous Phase: Synthesis, DFT Calculations, and Enhanced Antibacterial Activities

To explore the interactions of nanoparticles and bioresources and elucidate their effects on the morphology of the resulting composite, hierarchically structured cellulose@ZnO composites have been synthesized by an environmentally friendly hydrothermal method in one step. First, self-assembly induces the formation of hierarchical three-level structures, including cellulose/ZnO nanofibers, layers, and microfibers. Then, ZnO microparticles deposit onto the surface of the third-level cellulose/ZnO microfibers and accomplish the fabrication of a cellulose@ZnO composite, which eventually defines the hierarchical morphology of synthesized materials. The self-assembly mechanism was comprehensively examined. The electrostatic attraction between cellulose and ZnO, not hydrogen bonding, was found to be the main driving force for the formation of the first-level structure. A density functional theory study was conducted to support the self-assembly mechanism by optimizing the cellulose/ZnO structures at the molecular level, computing the corresponding thermodynamic energies and examining the spectroscopic properties. A hierarchically structured cellulose@ZnO composite is found to enhance the antibacterial activities. The diameters of the inhibition zone were found to be 48.8 and 45.5 mm against the Gram-positive bacterium Staphylococcus aureus ( S. aureus ) and the Gram-negative bacterium Escherichia coli ( E. coli ), respectively. This study is expected to improve food packaging materials while utilizing our newly synthesized cellulose@ZnO composite.