Octylamine-Modified Cellulose Nanocrystal-Enhanced Stabilization of Pickering Emulsions for Self-Healing Composite Coatings

[Image: see text] Linseed oil-in-water Pickering emulsions are stabilized by both sulfated CNCs (sCNCs) and octylamine-modified CNCs (oCNCs). oCNCs with hydrophobic moieties grafted on the surfaces of otherwise intact nanocrystals provided emulsions exhibiting stronger resistance to creaming of oil droplets, compared with unmodified sCNCs. sCNCs were not able to completely stabilize linseed oil in water at low CNC concentrations while oCNCs provided emulsions with no unemulsified oil residue at the same concentrations. Oil droplets in oCNC emulsions were smaller than those in samples stabilized by sCNCs, corresponding with an increased hydrophobicity of oCNCs. Cryo-SEM imaging of stabilized droplets demonstrated the formation of a CNC network at the oil–water interface, protecting the oil droplets from coalescence even after compaction under centrifugal force. These oil droplets, protected by a stabilized CNC network, were dispersed in a water-based commercial varnish, to generate a composite coating. Scratches made on these coatings self-healed as a result of the reaction of the linseed oil bled from the damaged droplets with oxygen. The leakage and drying of the linseed oil at the location of the scratches happened without intervention and was accelerated by the application of heat.