A flexible, hydrophobic, and multilayered poly(vinyl alcohol) (PVA) film evolved to replace a commercially available nonbiodegradable easy seal-paper (ES-PAPER) sealing film. First, environmentally friendly fillers, such as cellulose nanocrystals (CNCs) or cellulose nanofibers (CNFs), were added to produce PVA + CNC/CNF composites via blade coating and solution casting to strengthen the mechanical properties of PVA. Subsequently, biodegradable and hydrophobic materials, such as poly(ethylene glycol)-poly(lactic acid) (PEG-PLA) and neat PLA, were added to prepare multilayered PEG-PLA and PLA hydrophobic composites using double-sided solution casting. The hydrophobicity of PVA was enhanced through heat treatment. Finally, the mechanical properties of the as-prepared PVA film were compared with those of a commercially available ES-PAPER sealing film. PVA + CNC/CNF composites exhibit excellent transparency and mechanical properties, whereas PVA + CNCs 3.0 wt% have the highest Young's modulus and tensile strength, which are, respectively, 3% and 96% higher than the Young's modulus and tensile strength of an ES-PAPER sealing film. With regard to strain at break, the prepared PVA film also exhibited a value many times larger than that of the ES-PAPER sealing film because of good filler dispersibility, which significantly enhanced the durability of the sealing film.
Keywords: Multilayered; cellulose; hydrophobic; poly(vinyl alcohol); sealing film.