High throughput disassembly of cellulose nanoribbons and colloidal stabilization of gel-like Pickering emulsions

Abstract

We introduce a strategy to disintegrate cellulose microfibrils present in the cell walls of plant fibers. The process includes impregnation and mild oxidation followed by ultrasonication, which loosens the hydrophilic planes of crystalline cellulose while preserving the hydrophobic ones. The resultant molecularly-sized cellulose structures (cellulose ribbons, CR) retain a length of the order of a micron (1.47 ± 0.48 μm, AFM). A very high axial aspect ratio is determined (at least 190), considering the CR height (0.62 ± 0.38 nm, AFM), corresponding to 1-2 cellulose chains, and width (7.64 ± 1.82 nm, TEM). The new molecularly-thin cellulose proposes excellent hydrophilicity and flexibility, enabling a remarkable viscosifying effect when dispersed in aqueous media (shear-thinning, zero shear viscosity of 6.3 × 10⁵ mPa·s). As such, CR suspensions readily develop into gel-like Pickering emulsions in the absence of crosslinking, suitable for direct ink writing at ultra-low solids content.

Keywords: Cellulose; Direct ink writing (DIW); Molecularly thin cellulose ribbons; Nanocellulose; Pickering emulsions.