Surface Structuring and Water Interactions of Nanocellulose Filaments Modified with Organosilanes toward Wearable Materials

[Image: see text] Colloidal dispersions of cellulose nanofibrils (CNFs) are viable alternatives to cellulose II dissolutions used for filament spinning. The porosity and water vapor affinity of CNF filaments make them suitable for controlled breathability. However, many textile applications also require water repellence. Here, we investigated the effects of postmodification of wet-spun CNF filaments via chemical vapor deposition (CVD). Two organosilanes with different numbers of methyl substituents were considered. Various surface structures were achieved, either as continuous, homogeneous coating layers or as three-dimensional, hairy-like assemblies. Such surface features reduced the surface energy, which significantly affected the interactions with water. Filaments with water contact angles of up to 116° were obtained, and surface energy measurements indicated the possibility of developing amphiphobicity. Dynamic vapor sorption and full immersion experiments were carried out to inquire about the interactions with water, whether in the liquid or gas forms. Mechanical tests revealed that the wet strength of the modified filaments were almost 3 times higher than that of the unmodified precursors. The hydrolytic and mechanical stabilities of the adsorbed layers were also revealed. Overall, our results shed light on the transformation of aqueous dispersions of CNFs into filaments that are suited for controlled interactions with water via concurrent hydrolysis and condensation reactions in CVD, while maintaining the moisture buffering capacity and breathability of related structures.