All-natural chitosan-based polyimine vitrimer with multiple advantages: A novel strategy to solve nondegradable plastic waste pollution.

The increasing amount of nondegradable petroleum-based plastic waste releases chemical hazards, posing a significant threat to the environment and human health. Chitosan, derived from marine wastes, is an attractive feedstock for the preparation of plastic replacement due to its renewable and degradable nature. However, in most cases, complex chemical modifications of chitosan or hybridization with chemicals from fossil resources are required. Herein, we present a high-performance chitosan-based polyimine vitrimer (CS-PI) through a mild and catalyst-free Schiff base reaction between chitosan and vanillin. The CS-PI were formed by integrating dynamic imine bonds into the polymer networks, resulting in superior thermo-processability and mechanical performances. The tensile strength and Young's modulus of the CS-PI films reached 38.72 MPa and 3.20 GPa, respectively, which was significantly higher than that of both commercial petroleum-based plastics and bioplastics. Additionally, the CS-PI films exhibited good light transmittance, self-healing ability, reprocess capacity, water resistance, and durability to various organic solvents. Moreover, the CS-PI films could be completely degraded under both acidic and natural conditions, enabling a sustainable circulation. Therefore, this work offers a new design strategy for developing all-natural environmentally friendly polymers as sustainable replacements for petroleum-based plastics, thus reducing the accumulation of nondegradable plastic waste.