Structural and Morphological Features of Anisotropic Chitosan Hydrogels Obtained by Ion-Induced Neutralization in a Triethanolamine Medium

Abstract

For the first time, anisotropic hydrogel material with a highly oriented structure was obtained by the chemical reaction of polymer-analogous transformation of chitosan glycolate—chitosan base using triethanolamine (TEA) as a neutralizing reagent. Tangential bands or concentric rings, depending on the reaction conditions, represent the structural anisotropy of the hydrogel. The formation kinetics and the ratio of the positions of these periodic structures are described by the Liesegang regularities. Detailed information about the bands is given (formation time, coordinate, width, height, and formation rate). The supramolecular ordering anisotropy of the resulting material was evaluated both by the number of Liesegang bands (up to 16) and by the average values of the TEA diffusion coefficient ((15–153) × 10−10 and (4–33) × 10−10 m2/s), corresponding to the initial and final phase of the experiment, respectively. The minimum chitosan concentration required to form a spatial gel network and, accordingly, a layered anisotropic structure was estimated as 1.5 g/dL. Morphological features of the structural anisotropic ordering of chitosan Liesegang structures are visualized by scanning electron microscopy. The hemocompatibility of the material obtained was tested, and its high sorption–desorption properties were evaluated using the example of loading–release of cholecalciferol (loading degree ~35–45%, 100% desorption within 25–28 h), which was observed for a hydrophobic substance inside a chitosan-based material for the first time.