Development of Cellulose Nanocrystal (CNC)-Reinforced PLA/PMMA Nanocomposite Coatings for Sustainable Paper-Based Packaging

Driven by environmental concerns, the packaging industry is shifting toward high-performance and bio-based coating alternatives. In this research, poly(methylmethacrylate) (PMMA) and modified cellulose nanocrystal (m-CNC) were employed as reinforcing agents to develop sustainable poly (lactic acid)-based coatings for packaging applications. Various formulations, influenced by polymer matrix blends and m-CNC loadings (1-5%), were prepared using solvent and applied as protective coating on cardboard paper substrates. The grammage of polymeric coatings (CG) on paper was also investigated using various wet film thicknesses (i.e., 150-250 μm). Accordingly, key parameters including water contact angle, thermal behavior, mechanical performances and barrier properties were systematically evaluated to assess the effectiveness of the developed nanocomposite coatings. As a result, nonylphenol ethoxylate surfactant-modified cellulose nanocrystals exhibited good dispersion and stable suspension in chloroform for one hour, improving compatibility and interaction of polymer-CNC fillers. The water vapor permeability (WVP) of PLA-coated papers was significantly reduced by blending PMMA and increasing the content of m-CNC nanofillers. Furthermore, CNC incorporation enhanced the oil resistance of PLA/PMMA-coated cardboard. Pronounced improvements in barrier properties were observed for paper substrates coated with dry coat weight or CG of ~20 g/m² (corresponding to 250 μm wet film thickness). Coatings based on blended polymer-particularly those reinforced with nanofillers-markedly enhanced the hydrophobicity of the cardboard papers. SEM-microscopy confirmed the structural integrity and morphology of the nanocomposite coatings. Regarding mechanical properties, the upgraded nanocomposite copolymer (PLA-75%/PMMA-25%/m-CNC3%) exhibited the highest bending test and tensile strength, achieved on coated papers and free-standing polymeric films, respectively. Based on DSC analysis, the thermal characteristics of the PLA matrix were influenced to some extent by the presence of PMMA and m-CNC. Overall, PLA/PMMA blends with an optimal amount of CNC nanofillers offer promising sustainable coatings for the packaging applications.