New monolithic nanocomposite silica biomaterials were synthesized on the basis of various natural polysaccharides and recently introduced completely water-soluble precursor tetrakis(2-hydroxyethyl) orthosilicate. The sol-gel processes were performed in aqueous solutions without the addition of organic solvents and catalysts. The silica polymerization was promoted by the polysaccharides through acceleration and catalytic effect on the processes. By introducing poly(vinyl alcohol) or poly(ethylene oxide) in the precursor solution, it was shown that the jellification took place in the case of the hydroxyl-containing polymer. Therefore, it was suggested that the catalysis was caused by a formation of hydrogen bonds between hydroxyl groups in macromolecules and products of precursor hydrolysis (silanols). It was also demonstrated that the polysaccharides radically changed the structure of biomaterials. In place of the cross-linked nanoparticles, there was a three-dimensional network from crossed or branched fibers and uncrossed spherical particles that filled the mesh space. The density of network, thickness of fibers, and properties of synthesized biomaterials depended on the polysaccharide type, charged degree of their macromolecule, and concentration. By varying these parameters, it was possible to manipulate the structural organization of hybrid polysaccharide-silica nanocomposites.
Bionanocomposites are a novel class of nanosized materials. They contain the constituent of biological origin and particles with at least one dimension in the range of 1–100 nm. There are similarities with nanocomposites but also fundamental differences in the methods of preparation, properties, functionalities, biodegradability, biocompatibility, and applications. The article includes two parts. Bionanocomposite definition and classification along with nanoparticles, biomaterials, and methods of their preparation are initially reviewed. Then, novel approaches developed by our team are presented. The first approach concerns the preparation of bionanocomposites from chitosan and nanoparticles. It is based on the regulated charging of polysaccharide by the gradual shift of solution pH. When charges appear, the biomacromolecules come into the electrostatic interactions with negatively charged nanoparticles that cause the jellification of solutions. It is also applied to form films. They have a nacre-like structure from stacked planar nanoparticles separated by aligned biomacromolecules. The second approach deals with the biomimicking mineralization of biopolymers by using a novel silica precursor. Its advantage over the current sol-gel processing is in the compatibility and regulation of processes and structure of generated silica. Another example of the mineralization is presented by titania. Syntheses are performed in anhydrous ethylene glycol. Processes and structure of bionanocomposites are regulated by water that is added in an amount to only hydrate functional groups in the carbohydrate macromolecule.
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