Ozone was used as a green and environmentally friendly initiator to directly induce a Schiff base cross-linking reaction between chitosan and waxy rice starch (CS) in the present investigation. The effects of oxidation on the structure of chitosan/starch bio-based composite, along with the cross-linked structure formation via Schiff base reaction, were investigated and confirmed using FTIR, XRD, and XPS characterization techniques. The formation of new bonds (C=N) along with other attributes imparted by the cross-linking reaction were evaluated and characterized. Notably, the ozone-induced cross-linking reaction significantly altered the water retention capabilities of CS, especially in the case of aqueous ozone treatment, which significantly improved its swelling power, water holding capacities, and water adsorption. Additionally, aqueous ozone treatment facilitated the formation and stabilization of the gel network. Gaseous ozone in dry state proved more effective in promoting the formation of CN groups, leading to enhanced surface hydrophobicity, while aqueous ozone offered better oxidation uniformity for the coexistence system of chitosan and starch. This work provides a novel and environmentally friendly approach for fabricating the chitosan/starch chemically cross-linking materials through ozone-induced direct Schiff base reaction, which simplifies the preparation process of the complex and minimizing the utilization of solvents.
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