Layer-by-layer assembled graphene oxide/polydiallydimethylammonium chloride composites for hydrogen gas barrier application

Poly(diallyldimethylammoium chloride) (PDDA)/acid or base modified graphene oxide (MGO) composite (PDDA/MGO)-based gas barrier films were prepared by layer-by-layer (LBL) assembly method on polyethylene terephthalate (PET) substrate using a spray coating assisted deposition. The effect of pH on the hydrogen gas permeability (H₂GP) values of the different MGO-based films was investigated to determine the optimum pH value of the MGO solution for the preparation of PDDA/MGO-based LBL assembly. Accordingly, the different numbers of bilayers based LBL-assembled films were prepared using alternate deposition of PDDA and MGO solutions and the H₂GP values were measured for those assemblies. The films were characterized by XRD, FT-IR, and Raman spectroscopy analyses. The morphology of the LBL-assembled film was observed by cross-sectional field emission scanning electron microscopy which confirms densely packed layered structure. The H₂GP of six bilayers PDDA/MGO composite film is 5.7 cc/m²⋅d⋅atm, which is much lower than that of pure PET substrate (170.7 cc/m²⋅d⋅atm), indicating 96.7% decrease in H₂GP. This result suggests that the PDDA/MGO composite film could be used as a potential candidate to fabricate hydrogen gas barrier coating material.