The harm caused by small rubber particles generated from tire abrasion to the atmosphere is receiving a continuing concern. For developing environmental-friendly tire tread materials with high wear resistance, building the strong interface between nano-fillers and rubber matrix is the primary challenge. Herein, ionic liquid (IL, 1-allyl-3-methylimidazole chloride) was used to modify graphene oxide (GO) by π-cation interaction and hydrogen bonding between IL and GO. Furthermore, an IL-GO/natural rubber (NR) masterbatch possessing fine dispersion of GO was prepared by the emulsion compounding method, and thereafter, a further compound with solution polymerized styrene butadiene rubber (SSBR) was fabricated for the tread rubber composite. Results showed that the double bond in the IL enhanced the crosslinking reaction during the vulcanization of rubber composites occurred at high temperature, leading to an elevated interfacial interaction between the IL-modified GO and the rubber macromolecules. Compared with silicon dioxide (SiO 2 )-filled NR/SSBR composites, the cross-link density, 300% modulus, and tear strength of the IL-GO/SiO 2 /NR/SSBR composites were increased by 10.2, 42.6, and 20.2%, respectively. Importantly, the wear resistance of the IL-GO/SiO 2 /NR/SSBR composites was improved by 17.3%, ascribing to the strong interface between IL-GO and rubber macromolecules.

High wear-resistance and fuel-saving tires play an important role in reducing the environmental pollution caused by automobiles. The filler dispersion and interfacial interactions are both crucial for affecting the wear and rolling resistances of rubber composites. In this study, the ionic liquid 1-aminopropyl-3-methylimidazolium chloride (IL–NH2) was specially selected to tune the surface characteristics of graphene oxide (GO), and then the modified GO (IL–NH2–GO) was further introduced to a natural rubber/solution-polymerized styrene–butadiene rubber (NR/SSBR) matrix to investigate the effects of the IL–NH2 dosage on the microstructure and properties of the IL–NH2–GO/NR/SSBR composites. The results showed that the filler dispersion and interface between the fillers and rubber macromolecules were enhanced by introducing an appropriate IL–NH2 content. Owing to the change in the chemical structure of the GO-surface and lubrication effect of the IL–NH2, the filler dispersion was obviously improved, and the friction was reduced between the GO and rubber macromolecules. When the IL–NH2-to-GO mass ratio was 1:1, the 100% modulus and tensile strength of the IL–NH2–GO/NR/SSBR increased by 18.5 and 7.8%, respectively, compared with those of the GO/NR/SSBR composites. Meanwhile, the wear and rolling resistances improved by 8.6% and decreased by 10.4%, respectively. This research indicates that the facile strategy developed for modifying GO with ionic liquids has promising potential for preparing eco-friendly tires exhibiting high wear and low rolling resistances.

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