We envision that dispersion between two polymeric materials on mesoscales would create new composites with properties that are much more superior to the components alone. Here we elucidate the dispersion between two of most abundant natural polysaccharides, starch and chitosan, which form mesoscale composites that may promise many applications. By using X-ray microscopic imaging, small-angle X-ray scattering, and differential scanning calorimetry, we were able to characterize the interactions of chitosan and starch in the mesoscale composites. The morphology of the composite is far more complex from the simple mixture of starch granules with a nominal size of a few micrometers and chitosan microbundles of tens and hundreds of micrometers. This unique morphology can only be explained by the enhanced miscibility of chitosan in a starch granular matrix. It is evidenced that there is a possible ionic interaction between the amino group in chitosan and the hydroxyl groups in starch granules. Despite the limited solubility of chitosan in water, this ionic interaction allows for the disassembly of chitosan microbundles within the starch suspension. The result is a chemically stronger and more stable granular composite formed by two biocompatible and biodegradable polysaccharide polymers. The mechanism of chitosan to disperse throughout starch granules has implications for the application of chitosan in water and other solvents.
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