Comparative Structure–Property Relationship between Nanoclay and Cellulose Nanofiber Reinforced Natural Rubber Nanocomposites

Natural rubber (NR) nanocomposites reinforced with five parts per hundred rubber (phr) of two different nano-fillers, i.e., nanoclay (abbrev. NC) and cellulose nanofiber (abbrev. CNF), were prepared by using latex mixing approach, followed by mill-compounding and molding. The morphology, stress–strain behavior, strain-induced crystallization, and bound rubber of the NR nanocomposites were systematically compared through TEM, tensile test, WAXS, DMA, and bound rubber measurement. The aggregated CNFs were observed in the NR matrix, while the dispersed nanosized clay tactoids were detected across the NR phase. The reinforcement effects of NC and CNF were clearly distinct in the NR nanocomposites. At the same nano-filler content, the addition of NC and CNF effectively accelerated strain-induced crystallization of NR. The high tensile strength obtained in the NC-filled NR nanocomposite was attributed to strain-induced crystallization of NR accelerated by well-dispersed NC. However, the larger tensile modulus and low strain for the CNF-filled NR were related to the formation of immobilized NR at the interface between CNF aggregate and NR. The immobilization effect of NR at the CNF surface offered by a mutual entanglement of CNF aggregate and NR chain led to local stress concentration and accelerated strain-induced crystallization of CNF/NR nanocomposite. From the present study, the NR nanocomposites combined with 5 phr CNF shows high-tensile modulus and acceptable breaking tensile stress and strain, suggesting the application of CNF/NR based nanocomposite in automotive and stretchable sensors for next-generation electronic devices