High strength chitosan-based nanocomposites with aligned nanosheets and crosslinked networks

High strength/toughness nanocomposites are increasingly in demand due to the development needs of high-end applications. However, the aggregation and random orientation of nanofillers and the weak crosslinking of the polymer matrix lead to the degradation of the mechanical properties of nanocomposites. Here, we present a strategy to prepare chitosan-based nanocomposites with aligned nanosheets via the in situ photo-crosslinking of modified chitosan. The well-dispersed and highly aligned nanosheets, as well as the dense covalently crosslinked network between the modified chitosan chains, effectively improve the mechanical properties of the prepared nanocomposites. For example, the chitosan-based nanocomposite films exhibit a tensile strength of up to 340.6 ± 13.4 MPa, a Young's modulus of 8.2 ± 0.2 GPa and a toughness of 22.0 ± 2.5 MJ m^-3, which are 4.2, 4.8 and 1.8 times higher, respectively, than those of pure chitosan films. Moreover, the thermal decomposition temperature of the chitosan-based nanocomposite films reaches 286.8 °C, which is 48.5 °C higher than that of pure chitosan films. We consider that our strategy, which constructs a crosslinked chitosan structure with aligned nanofillers, could lead to the development and application of the bio-based composites with excellent mechanical properties.