Natural Biodegradable Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Nanocomposites with Multifunctional Cellulose Nanocrystals/Graphene Oxide Hybrids for High-Performance Food Packaging.

High-performance and useful graphene oxide (GO) and cellulose nanocrystals (CNCs) are easily extracted from natural graphite and cellulose raw materials, and poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) is produced by bacterial fermentation from natural plant corn stalks, etc. In this study, novel ternary nanocomposites consisting of PHBV/cellulose nanocrystal-graphene oxide nanohybrids were prepared via a simple solution casting method. The synergistic effect of CNC with GO nanohybrids obtained by chemical grafting (CNC-GO, covalent bonds) and physical blending (CNC/GO, noncovalent bonds) on the physicochemical properties of PHBV nanocomposites was evaluated and the results compared with a single component nanofiller (CNC or GO) in binary nanocomposites. More interestingly, ternary nanocomposites displayed the highest thermal stability and mechanical properties. Compared to neat PHBV, the tensile strength and elongation to break increased by 170.2 and 52.1%, respectively, and maximum degradation temperature (Tmax) increment by 26.3 °C, were observed for the ternary nanocomposite with 1 wt % covalent bonded CNC-GO. Compared to neat PHBV, binary, and 1:0.5 wt % noncovalent CNC/GO based nanocomposites, the ternary nanocomposites with 1 wt % covalent bonded CNC-GO exhibited excellent barrier properties, good antibacterial activity (antibacterial ratio of 100.0%), reduced barrier properties, and lower migration level for both food simulants. Such a synergistic effect yielded high-performance ternary nanocomposites with great potential for bioactive food packaging materials.