Toward Sustainable Multifunctional Coatings Containing Nanocellulose in a Hybrid Glass Matrix

We report on a sustainable route to protective nanocomposite coatings, where one of the components, nanocellulose fibrils, is derived from trees and the glass matrix is an inexpensive sol–gel organic–inorganic hybrid of zirconium alkoxide and an epoxy-functionalized silane. The hydrophilic nature of the colloidal nanocellulose fibrils is exploited to obtain a homogeneous one-pot suspension of the nanocellulose in the aqueous sol–gel matrix precursors solution. The mixture is then sprayed to form nanocomposite coatings of a well-dispersed, random in-plane nanocellulose fibril network in a continuous organic–inorganic glass matrix phase. The nanocellulose incorporation in the sol–gel matrix resulted in nanostructured composites with marked effects on salient coating properties including optical transmittance, hardness, fracture energy, and water contact angle. The particular role of the nanocellulose fibrils on coating fracture properties, important for coating reliability, was analyzed and discussed in terms of fibril morphology, molecular matrix, and nanocellulose/matrix interactions.