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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 SiO 2 (Si-NH 2 ). Through strong hydrogen-bonding interaction between the phenolic hydroxyl groups on G-TA and primary amine groups on Si-NH 2 , SiO 2 was uniformly loaded to the surface of graphene. Due to the synergistic dispersion effect of graphene and SiO 2 , which prevents restacking and re-aggregating of both graphene and SiO 2 , HGS hybrids were distributed evenly in the natural rubber (NR) matrix (HGS@NR). Simultaneously, the surface roughness of graphene after loading SiO 2 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 SiO 2 (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-SiO 2 hybrid fillers has been established.

Synergistic effect of graphene and silicon dioxide hybrids through hydrogen bonding self-assembly in elastomer composites