Effect of a Montmorillonite Modification on the Rheology and Mechanical Properties of a Clay/Natural Rubber Nanocomposite

Clay/natural rubber (Clay–NR) nanocomposites are a sustainable material class with a wide range of applications. The type and amount of the filler added to the rubber matrix promote significant changes in the matrix properties. Montmorillonitic clays (MMT) are mineral, natural fillers. This study investigates the effect of a modified Brazilian polycationic MMT on the nanocomposite rheology and mechanical properties. The MMT was incorporated into a NR matrix in its natural state, and after modification by cation exchange (MMTNa) and organophilization (MMTORG), at concentrations of 2.5 and 5 phr (parts per hundred parts of rubber). The natural and modified clays were characterized by XRD, FTIR, BET, and SEM/EDS. Mechanical tests (tensile strength, elongation at break, and modulus at 100%) indicated that the use of MMTNa led to increased strength and modulus, whereas a minor decrease in the elongation was observed. However, the use of MMTORG yielded the most significant improvements in the mechanical properties. The rheology tests indicated that the Payne effect was not observed, and the strain-dependent behavior arises from matrix-dominated mechanisms, rather than disruption of a filler network. Vulcanization curves showed that the NR-MMTORG composites exhibited higher torque values, corroborated by higher crosslink densities. These findings highlight the critical role of cation exchange modification in optimizing MMT dispersion and interfacial interactions within NR matrices, providing design principles for high-performance sustainable nanocomposites.