AbstractBlends of natural rubber (NR)/chlorobutyl rubber (CIIR) (50/50), along with their nanocomposites containing varying amounts of graphene nanoparticles (GNPs) with and without silane, were prepared using different feeding sequences and mixers. The results indicated that when GNP was first mixed with NR before adding CIIR, the highest GNP content was found in NR; the oxygen permeability and diffusion coefficient decreased significantly by 37% and 55%, respectively. Conversely, when graphene was initially added to CIIR, it was distributed in both rubbers and at the interface, enhancing phase interaction and achieving a finer morphology. This sample exhibited the greatest improvement in mechanical properties due to specific localization of GNP and increased crosslink density. Using an internal mixer instead of a two‐roll mill improved graphene dispersion, reduced curing time, and enhanced mechanical properties. Although the presence of silane reduced graphene dispersion, it improved mechanical and barrier properties due to increased crosslink density. Oxygen permeability was reduced by up to 36% at 3 phr of GNP content with silane. This research proves that the mixing order and the type of mixing equipment are crucial in determining the final performance of rubber composites, as they significantly influence the dispersion and localization of fillers.Highlights NR/CIIR/GNP nanocomposites were prepared by different methods and evaluated. Adding NR/GNP to CIIR led to more presence of GNP in NR and lower permeability. By adding CIIR/GNP to NR, GNP were placed more at interface, modulus improved. Mixing in an internal mixer improved GNP dispersion compared to a two‐roll mill. Silane improved mechanical and barrier properties of NR/CIIR/GNP nanocomposite.
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