Elastomer nanocomposites filled with graphene-based nanomaterials: insights from molecular dynamics simulations

Abstract Elastomers are a class of polymers known for their elasticity and resilience, widely used in various industries. However, their application is limited by insufficient mechanical performance, including low stiffness, poor wear resistance and barrier properties. Therefore, elastomers are typically reinforced with fillers to enhance their durability, mechanical performance, and functional properties. The rapid advancements in nanotechnology have led to the exploration of graphene-based nanomaterials (GNMs), such as graphene and graphene oxide (GO), as potential fillers to enhance the properties of elastomers. While several reviews have summarised experimental advances in GNMs filled elastomer nanocomposites, a comprehensive review focused specifically on insights from computational modelling remains limited. This review addresses this gap by critically synthesising theoretical studies of GNMs–elastomer nanocomposites, with emphasis on interfacial interaction mechanisms, compatibility and dispersion, mechanical and tribological properties, thermal transport, barrier properties, and importance of appropriate force field selection and validation. Common elastomer matrices, including natural rubber, styrene-butadiene rubber, nitrile-butadiene rubber, and thermoplastic polyurethane, are discussed, and simulation findings are compared with experimental observations to highlight agreements, discrepancies, and limitations. Overall, this review provides a molecular-level framework for understanding how GNMs structure and elastomer chemistry govern interfacial interactions, and how these interactions determine the mechanical, tribological, thermal, and barrier properties of high-performance elastomer nanocomposites.