Nanocellulose Grades with Different Morphologies and Surface Modification as Additives for Waterborne Epoxy Coatings.

While adding different micro- and nanocellulose types into epoxy coating formulations with waterborne phenalkamine crosslinker, effects on processing conditions and coating performance were systematically investigated. The variations in viscosity, thermal and thermomechanical properties, mechanical behavior, abrasive wear, water contact angles, and coating morphologies were evaluated. The selected additives include microcrystalline cellulose (MCC) at 1 to 10 wt.% and cellulose nanocrystals (CNC), cellulose nanofibers (CNF), cellulose microfibers (CMF), and hydrophobically modified cellulose microfibers (mCMF) at 0.1 to 1.5 wt.%. The viscosity profiles are determined by the inherent additive characteristics with strong shear thinning effects for epoxy/CNF, while the epoxy/mCMF provides lower viscosity and better matrix compatibility owing to the lubrication of encapsulated wax. The crosslinking of epoxy/CNF is favored and postponed for epoxy/(CNC, CMF, mCMF), as the stronger interactions between epoxy and CNF are confirmed by an increase in the glass transition temperature and reduction in the dampening factor. The mechanical properties indicate the highest hardness and impact strength for epoxy/CNF resulting in the lowest abrasion wear rates, but ductility enhances and wear rates mostly reduce for epoxy/mCMF together with hydrophobic protection. In addition, the mechanical reinforcement owing to the specific organization of a nanocellulose network at percolation threshold concentrations of 0.75 wt.% is confirmed by microscopic analysis: the latter results in a 2.6 °C (CNF) or 1.6 °C (CNC) increase in the glass transition temperature, 50% (CNF) or 20% (CNC) increase in the E modulus, 37% (CNF) or 32% (CNC) increase in hardness, and 58% (CNF) or 33% (CNC) lower abrasive wear compared to neat epoxy, while higher concentrations up to 1.5 wt.% mCMF can be added. This research significantly demonstrates that nanocellulose is directly compatible with a waterborne phenalkamine crosslinker and actively contributes to the crosslinking of waterborne epoxy coatings, changing the intrinsic glass transition temperatures and hardness properties, to which mechanical coating performance directly relates.