Robust Oil-Fouling Resistance of Amorphous Cellulose Surface Underwater: A Wetting Study and Application

The antioil-fouling characteristic of an amorphous cellulose (a-cellulose) surface was elucidated using the sessile droplet method (static) and a modified Wilhelmy plate technique (dynamic). As compared to other hydrophilic surfaces (cellulose acetate, poly(vinyl alcohol), and glass), the oil (poly(dimethylsiloxane)) contact angle on the a-cellulose surface underwater shows the largest value (170.5 ± 5.0°), having the smallest deviation from its theoretical value (180.0°) as estimated by Young's equation. Also, the a-cellulose surface demonstrates the strongest affinity with water in an oil medium (stable hydrophilicity). Moreover, the work of adhesion between the receding oil phase and a-cellulose underwater is quantified to be 10.3 mN/m, approximately one-fourth of that in air (42.0 mN/m). The overall wetting study suggests a rather low oil/solid/water three-phase contact line (TPL) friction in the direction that water displaces oil. A proposed mechanism attributes these phenomena to the water-accessible rigid cellulose chains and supramolecular structure of a-cellulose. The former hinders molecular rearrangement during processing or upon exposure to oil, such that its polar hydroxyl groups are readily accessible to water, thereby retaining its hydrophilicity. The latter allows water to diffuse across the TPL, forming the hydration shells that weaken the van der Waals interactions between oil and cellulose chains. Such findings of the a-cellulose surface can be exploited to fabricate mesh membranes with high water permeation flux (375.4 ± 13.5 L m^-2 h^-1 Pa^-1), high oil/water separation efficiency (93-98%), and long-lasting stability, which is suitable for offshore oil spill remediation.