Fabrication and Characterization of Hydrophobic Cellulose Nanofibrils/Silica Nanocomposites with Hexadecyltrimethoxysilane

Cellulose nanofibrils (CNFs) have attracted much attention because of their renewability and potential biocompatibility. However, CNFs are extremely hydrophilic due to the presence of a large number of hydroxyl groups, limiting their use as a water-resistant material. In this work, we controlled the adsorption behavior of silica nanoparticles on the surface of CNFs by adjusting the synthesis conditions. The silica nanoparticle size and packing efficiency on the CNF surface could be controlled by varying the ammonium hydroxide and water concentrations. In addition, hexadecyltrimethoxysilane (HDTMS) was successfully grafted onto CNF or CNF/silica nanocomposite surfaces, and the quantitative content of organic/inorganic substances in HDTMS was analyzed through XPS and TGA. The HDTMS-modified CNF/silica nanocomposites were more advantageous in terms of hydrophobicity than the HDTMS-modified CNF composites. This is because the silica nanoparticles were adsorbed on the surface of the CNFs, increasing the surface roughness and simultaneously increasing the amount of HDTMS. As a result, the HDTMS-modified CNFs showed a water contact angle (WCA) of ~80°, whereas HDTMS-modified CNF/silica nanocomposites obtained superhydrophobicity, with a WCA of up to ~159°. This study can provide a reference for the expansion of recyclable eco-friendly coating materials via the adsorption of silica nanoparticles and hydrophobic modification of CNF materials.