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Fillers are indispensable for rubber composites. Carbon black as an efficient reinforcing filler is most widely used in the rubber industry. However, the utilization of nonrenewable feedstock, energy consumption, and footprint for making carbon black lead to the seeking of alternative substitutes for carbon black, which is of great significance. Here in this work, the possibility of illite, a most common mineral in sedimentary rocks, as an alternative filler for natural rubber (NR) is determined. It is found that pristine illite slows the curing rate and decreases the cross-linking density of NR, which results in the inferior performance of NR. This is associated with the weak filler–rubber interaction, which is a vital factor in deciding the performance of rubber composites. Therefore, illite has been modified using hexadecyl trimethyl ammonium bromide (CTAB), a commonly used cation surfactant, for improving the filler–rubber interaction. The thus obtained C-illite is confirmed to be efficient for (i) enhancing the illite–NR interaction, (ii) improving the dispersion of illite in the NR matrix, and (iii) accelerating the curing process of NR with increased cross-linking density. All of these lead to significantly improved mechanical properties and wear resistance of the C-illite/NR composites, e.g., a 71.88% increase of the modulus at 300% strain compared to the pure NR and a 23.79% reduction of the DIN abrasion volume compared to the NR filled with 40 phr pristine illite. This illustrates the high possibility of CTAB-modified illite with an optimal particle size as a promising alternative filler of carbon black for reinforcing rubbers.

To achieve the sustainable development of the rubber industry, the substitute of carbon black, the most widely used but non-renewable filler produced from petroleum, has been considered one of the most effective ways. The naturally occurring illite with higher aspect ratio can be easily obtained in large amounts at lower cost and with lower energy consumption. Therefore, the expansion of its application in advanced materials is of great significance. To explore their potential use as an additive for reinforcing rubber, styrene butadiene rubber (SBR) composites with illites of different size with and without 3-mercaptopropyltriethoxysilane (KH580) modification were studied. It was found that the modification of illite by KH580 increases the K-illite/SBR interaction, and thus improves the dispersion of K-illite in the SBR matrix. The better dispersion of smaller size K-illite with stronger interfacial interaction improves the mechanical properties of SBR remarkably, by an increment of about nine times the tensile strength and more than ten times the modulus. These results demonstrate, except for the evident effect of particle size, the great importance of filler–rubber interaction on the performance of SBR composites. This may be of great significance for the potential wide use of the abundant naturally occurring illite as substitute filler for the rubber industry.

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