LAUSR

Abstract Hydrophobically modified chitosan (HMC) self-assembles in solution to form gels, making it suitable for applications in oil dispersion, hydrogel design and wound dressing. The self-assembly of HMC is driven by the association of hydrophobic moieties that are attached to chitosan monomers along the polymer chain. We present the results of discontinuous molecular dynamics simulations aimed at understanding how the length and density of the hydrophobic modification chains attached to HMC affect self-assembly and the structure of the resulting network. Long modification chains are required to promote the formation of a stable network in solution at a modification density of 5%; the networks form more readily at a modification density of 10%. The pore size distribution of the resulting HMC network is relatively independent of the modification chain length and density. Insertion of different sized hydrophobic nanoparticles into HMC has a significant impact on network formation, with the particles acting as junction points that promote the association of several HMC chains. The networks form faster in the presence of many small nanoparticles than in the presence of few large nanoparticles. We conclude that HMC could be a viable candidate to form hydrogels in solution.