Stabilization of Oil-in-Water Pickering Emulsions by Surface-Functionalized Cellulose Hydrogel

An amphiphilic cellulose (<b>CLH</b>) hydrogel was synthesized via grafting of quaternary ammonium groups onto cellulose. The structural properties of <b>CLH</b> were characterized via Fourier transform infrared (FTIR)/¹³C solid-state NMR spectroscopy, elemental (CHN) analysis, particle size distribution (PSD), thermogravimetric analysis (TGA), and wettability was assessed through contact angle measurements. Pickering emulsions of apolar oils in water were prepared using variable weights of the <b>CLH</b> hydrogel as the stabilizing agent, along with different methods of agitation (mechanical shaking and sonication). The characterization results for <b>CLH</b> provide support for the successful grafting of quaternary ammonium groups onto cellulose to produce hydrogels. Different methods of agitation of an oil/water mixture revealed the formation of an <i>oil-in-water</i> (O/W) Pickering emulsion that was stable to coalescence for over 14 days. The resulting emulsions showed variable droplet sizes and stability according to the dosage of <b>CLH</b> in the emulsion and the agitation method, where the emulsion droplet size is related to the particle size of <b>CLH</b>. The addition of methyl orange (MO), a probe to evaluate the phase partitioning of the dye, had minor effects on the emulsion droplet size, and the emulsion prepared with 0.8 wt.% of <b>CLH</b> and agitated via sonication exhibited the smallest droplet size and greatest stability. This study is anticipated to catalyze further research and the development of low-cost and sustainable biopolymer hydrogels as stabilizers for tunable Pickering emulsion. Grafted cellulose materials of this type represent versatile stabilizing agents for foods, agrochemicals, and pharmaceutical products and technologies.