Electrosterically stabilized nanocrystalline cellulose (ENCC) was modified in three ways: (1) the hydroxyl groups on C2 and C3 of glucose repeat units of ENCC were converted to aldehyde groups by periodate oxidation to various extents; (2) the carboxyl groups in the sodium form on ENCC were converted to the acid form by treating them with an acid-type ion-exchange resin; and (3) ENCC was cross-linked in two different ways by employing adipic dihydrazide as a cross-linker and water-soluble 1-ethyl-3-[3-(dimethylaminopropyl)] carbodiimide as a carboxyl-activating agent. Films were prepared from these modified ENCC suspensions by vacuum filtration. The effects of these three modifications on the properties of films were investigated by a variety of techniques, including UV-visible spectroscopy, a tensile test, thermogravimetric analysis (TGA), the water vapor transmission rate (WVTR), and contact angle (CA) studies. On the basis of the results from UV spectra, the transmittance of these films was as high as 87%, which shows them to be highly transparent. The tensile strength of these films was increased with increasing aldehyde content. From TGA and WVTR experiments, cross-linked films showed much higher thermal stability and lower water permeability. Furthermore, although the original cellulose is hydrophilic, these films also exhibited a certain hydrophobic behavior. Films treated by trichloromethylsilane become superhydrophobic. The unique characteristics of these transparent films are very promising for potential applications in flexible packaging and other high-technology products.
A novel biopolymer-based aerogel was developed by freeze-drying a hydrogel, synthesized from cross-linking bifunctional hairy nanocrystalline cellulose and carboxymethylated chitosan through a Schiff base reaction. The nanocelluloses, bearing aldehyde and carboxylic acid groups, facilitated the cross-linking with chitosan through imine bond formation while providing negatively charged functional groups, and chitosan was modified to accommodate carboxylic acid. The potential of this bioaerogel in environmental remediation was examined in a model system comprising methylene blue, a cationic dye. Electrostatic complexation between acidic groups on the anionic aerogel with the dye resulted in time-dependent dye adsorption, with long-time equilibrium dye concentration fitting well to the Langmuir isotherm, yielding a maximum adsorption capacity of ∼785 mg g and equilibrium constant K ∼ 0.0089 at room temperature. Dynamics of adsorption was modeled by numerically solving the unsteady-state diffusion-adsorption mass balance in a 1D spherical coordinate, which attested to a diffusion-controlled process with a Langmuir adsorption time constant τ ∼ 7.6 s. To the best of our knowledge, this bioaerogel exhibits the highest removal capacity as yet for any reusable adsorbents prepared from biopolymers. Successful adsorption-regeneration cycles proved an excellent reusability, and the adsorption capacity remained constant over a wide pH range (e.g., pH > 7). This work may pave the way toward ultralight green functional materials.
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