Bio-nanocomposites based on poly (vinyl alcohol) (PVA) and cellulosic nanostructures are favorable for active food packaging applications. The current study systematically investigates the mechanical properties, gas permeation, and swelling parameters of PVA composites with cellulose nanocrystals (CNC) or nano lignocellulose (NLC) fibers. Alterations in these macroscopic properties, which are critical for food packaging applications, are correlated with structural information at the molecular level. Strong interactions between the fillers and polymer host matrix were observed, while the PVA crystallinity exhibited a maximum at ~1% loading. Finally, the orientation of the PVA nanocrystals in the uniaxially stretched samples was found to depend non-monotonically on the CNC loading and draw ratio. Concerning the macroscopic properties of the composites, the swelling properties were reduced for the D1 food simulant, while for water, a considerable decrease was observed only when high NLC loadings were involved. Furthermore, although the water vapor transmission rates are roughly similar for all samples, the CO₂, N₂, and O₂ gas permeabilities are low, exhibiting further decrease in the 1% and 1–5% loading for CNC and NLC composites, respectively. The mechanical properties were considerably altered as a consequence of the good dispersion of the filler, increased crystallinity of the polymer matrix, and morphology of the filler. Thus, up to ~50%/~170% enhancement of the Young’s modulus and up to ~20%/~50% enhancement of the tensile strength are observed for the CNC/NLC composites. Interestingly, the elongation at break is also increased by ~20% for CNC composites, while it is reduced by ~40% for the NLC composites, signifying the favorable/unfavorable interactions of cellulose/lignin with the matrix.

Poly(ethylene oxide) (PEO)-based copolymers are at the forefront of advanced membrane materials for selective CO₂ separation. In this work, free-standing composite membranes were prepared by blending imidazolium-based ionic liquids (ILs) having different structural characteristics with a PEO-based copolymer previously developed by our group, targeting CO₂ permeability improvement and effective CO₂/gas separation. The effect of IL loading (30 and 40 wt%), alkyl chain length of the imidazolium cation (ethyl- and hexyl- chain) and the nature of the anion (TFSI^-, C(CN)₃^-) on physicochemical and gas transport properties were studied. Among all composite membranes, PEO-based copolymer with 40 wt% IL3-[HMIM][TFSI] containing the longer alkyl chain of the cation and TFSI^- as the anion exhibited the highest CO₂ permeability of 46.1 Barrer and ideal CO₂/H₂ and CO₂/CH₄ selectivities of 5.6 and 39.0, respectively, at 30 °C. In addition, almost all composite membranes surpassed the upper bound limit for CO₂/H₂ separation. The above membrane showed the highest water vapor permeability value of 50,000 Barrer under both wet and dry conditions and a corresponding H₂O/CO₂ ideal selectivity value of 1080; values that are comparable with those reported for other highly water-selective PEO-based polymers. These results suggest the potential application of this membrane in hydrogen purification and dehydration of CO₂ gas streams.