Supramolecular Chemistry-Driven Preparation of Nanostructured, Transformable, and Biologically Active Chitosan-Clustered Single, Binary, and Ternary Metal Oxide Bioplastics

Aside from their economical cost and resource depletion, petroleum-based plastics generate annually a substantial amount of waste with a negative and extremely alarming impact on the environment and public health. Consequently, rising interest was devoted to search for biobased materials to find sustainable alternatives. Herein, we report a new and straightforward method to incorporate endogenous nano-objects (exemplified herein by metal oxide clusters) within polysaccharide-based films. Supramolecular chemistry based on polysaccharide self-assembly associated with the sol-gel polymerization allowed converting soluble chitosan and metal alkoxide precursors to nanostructured chitosan-clustered metal oxide films. A broad range of discrete single, binary, and ternary mixed metal oxides was successfully incorporated in the resulting bioplastics. The multifaceted use of these films was demonstrated by transforming them under gentle thermal treatment to partially oxidized chitosan-metal oxide materials or by disintegrating them in aqueous conditions to yield stable, water-dispersed chitosan-coated-metal oxide nanoparticles. The utility of these functional films was demonstrated through their use as antimicrobial agents, where significant improvement for inhibiting growth of positive and negative bacteria was observed compared to native, nonmodified chitosan films.