Preparation of high‐performance and low‐rolling resistance tire tread compound based on hydrogen‐bonded self‐assembled graphene/carbon nanotube‐silica hybrid

Graphene/carbon nanotubes and silica hybrids (CTGS) with high dispersion and strong interface were prepared by hydrogen bond self‐assembly technique using green modifiers Tween‐80 (TW) and Oleylamine (YA) as “molecular bridge.” CTGS was added into natural rubber (NR) as an effective functional filler to prepare high‐performance, low‐rolling resistance, and antistatic tire tread. In the vulcanization process of NR filled with CTGS (CTGS/NR), CTGS can participate in the rubber vulcanization, and co‐vulcanization is a catalyst for constructing the strong interfacial interactions between CTGS and rubber. The extreme dispersion of CTGS hybrid in NR and the strong interfacial interaction between CTGS and NR are the basis for obtaining excellent comprehensive properties of CTGS/NR composites. The results show that compared with NR filled with silica modified by triethoxysilyl propyldisulfide (ST@SiO2/NR), NR filled with carbon nanotubes and silica hybrid (CTGS4) using YA as the molecular bridge (CTGS4/NR) has the best comprehensive performance. Its tensile strength increased from 27.41 to 30.18 MPa, increasing by 10.1%, the rolling resistance decreased from 0.098 to 0.087, decreasing by 11.2%, and the conductivity increased by three orders of magnitude (increasing from 2.321 × 10−7 S∙m−1 to 4.111 × 10−5 S∙m−1) indicating excellent electrostatic conductivity for CTGS hybrid with carbon nanotubes loading as low as 0.6 wt%. CTGS hybrid is expected to be a new functional filler for rubber, especially good for green tires with high‐performance, low‐rolling resistance, and antistatic performances.