Temperature‐dependent tribological and interfacial properties of perfluoroelastomer nanocomposites modified with graphene nanosheets functionalized through molecular dynamics simulations

Abstract The present simulation‐based study aims to develop high‐performance polymer nanocomposites (FFKM) by investigating the influence of graphene modified with different polar functional groups on the high‐temperature load‐bearing tribological and interfacial properties of FFKM nanocomposites. Molecular dynamics simulations were employed to explore the effects of hydroxyl (OH), carboxyl (COOH), and amino (NH2) functional groups on the tribological and interfacial behavior of FFKM across a broad temperature range (298–573 K). Utilizing analysis tools such as large‐scale atomic/molecular massively parallel simulator (CVFF, AIREBO and EAM), BIOVIA Materials Studio (2020), OVITO, and VMD, it was determined that the friction coefficient of FFKM composites decreases nonlinearly with increasing temperature. The polarity and hydrogen bonding capacity of the functional groups enhance intermolecular interactions, thereby further influencing the tribological response. The COOH‐GN/FFKM composite, with a surface roughness of 1.0352, resulted in substandard transfer film quality, diminished actual contact area, and elevated micro‐asperities, thereby fostering mechanical interlocking. Moreover, the surface roughness of functionalized graphene was found to augment the free volume of the composite and exhibited a positive correlation with pullout force. In conclusion, it can be stated that surface roughness exerts a significant influence on the tribological and interfacial properties of FFKM composites. Highlights Functionalized graphene enhances perfluoroelastomer's tribological performance. Polar groups increase interaction strength and reduce wear at high temperatures. Glass transition temperature varies with functional group type. Surface roughness significantly impacts friction and wear behavior.