Oxygen-Content-Dependent Interfacial and Barrier Effects of Graphene Fillers in PVA Adhesives Toward Durable...

Waterborne poly(vinyl alcohol) (PVA) adhesives are widely used in iodine-based polarizers, owing to their excellent transparency and interfacial adhesion. However, the intrinsic hydrophilicity of PVA compromises the long-term durability of polarizers under humid conditions. Herein, graphene derivatives with tunable oxygen contents and graphitization degrees, including graphene oxide (GO), partially reduced graphene oxide (rGO), and graphene nanosheets (GNs), were incorporated into a PVA/PEI adhesive system to investigate the oxygen-content-dependent interfacial interactions and moisture-barrier mechanisms. Structural analyses reveal that oxygen-rich GO enhances interfacial hydrogen bonding and polymer-graphene interactions, whereas highly graphitized GN primarily functions through its intrinsic lamellar barrier effect by increasing diffusion tortuosity and reducing water affinity. The rGO exhibits a compromise between interfacial interactions and barrier effects due to its moderate oxygen content and preserved graphene structure. Among them, the GN-modified adhesive demonstrates the most favorable overall performances, achieving a 14.71% reduction in the water vapor transmission rate (WVTR) of the assembled polarizer, enhanced moisture resistance, and improved antistatic capability while maintaining acceptable optical transparency. Furthermore, practical polarizer evaluations confirm that GN effectively suppresses moisture penetration, with only slight bubbling observed after 8 days of water immersion and no delamination or polarization degradation during a 40-day immersion test. These findings provide insights into the relationship between graphene oxygen content, interfacial interactions, and moisture-barrier behavior, offering an effective strategy for designing durable multifunctional waterborne adhesives for advanced optoelectronic polarizer applications.