A novel graphene-silicon dioxide hybrid (HGS) was prepared by plant polyphenol-tannic acid (TA) functionalized pristine graphene (G-TA) and primary amine-containing silane coupling agent modified SiO2 (Si-NH2). Through strong hydrogen-bonding interaction between the phenolic hydroxyl groups on G-TA and primary amine groups on Si-NH2, SiO2 was uniformly loaded to the surface of graphene. Due to the synergistic dispersion effect of graphene and SiO2, which prevents restacking and re-aggregating of both graphene and SiO2, HGS hybrids were distributed evenly in the natural rubber (NR) matrix (HGS@NR). Simultaneously, the surface roughness of graphene after loading SiO2 and the interfacial interaction between the HGS hybrid and NR matrix were substantially improved. Due to the good dispersion and strong interface, the overall properties of HGS@NR nanocomposites are drastically enhanced compared with those of GS@NR nanocomposites prepared by dispersing the blend of unmodified graphene and SiO2 (GS) in NR. The HGS@NR nanocomposites possess the highest tensile strength up to 27.8 MPa at 0.5 wt% and tear strength of 60.2 MPa at 0.5 wt%. Thermal conductivities of the HGS@NR nanocomposites were found to be 1.5-fold better than that of the GS@NR nanocomposites. Also, the HGS@NR nanocomposites exhibit excellent abrasive resistant capacity that is nearly 2-fold better than that of the GS@NR nanocomposites. These results suggest that HGS has great potential in high-performance nanocomposites and a new strategy of constructing the efficient graphene-SiO2 hybrid fillers has been established.
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