Bio-Composites of Polymyrcene Reinforced with Alkylamine-Grafted Graphene Oxide: Mechanical Properties of Sustainable Vulcanized Elastomers

Growing interest in developing sustainable materials that reduce dependence on fossil resources has led to increased development of bio-based elastomers that can compete with traditional materials in terms of performance when reinforced with additives. This study shows that functionalizing graphene oxide with different alkylamine chains (C8, C12, and C16) enables precise, multidimensional modulation of polymyrcene rubber (PMy) composite behavior. The main finding is that there is a critical concentration of ~1.5–2.0 phr and an optimal chain length of C16 that maximizes mechanical strength, elongation, and toughness simultaneously, thus avoiding the classic trade-off between stiffness and extensibility. Additionally, the study reveals biphasic behavior of graphene oxide modified with dodecylamine (GOA12) on curing kinetics. At low concentrations, GOA12 slows vulcanization by competing with accelerators, while at higher concentrations, it accelerates vulcanization via Zn–amine–sulfur complexes. This duality is reflected consistently in the crosslink density, Payne effect, and tensile properties, establishing a coherent structure–property correlation. Identifying an optimal crosslinking regime of ~8.5 × 10−4 mol/cm3 as the common denominator of the best formulations provides a rational design guide for high-performance elastomers based on renewable matrices and graphene-derived reinforcements. The decrease in tan δ observed through mechanical dynamic analysis suggests potential applications in the tire industry due to increased energy dissipation, which would improve fuel efficiency.