Abstract
To design the interface between carbon nanotubes and natural rubber (NR), a silane coupling agent, bis(3‐triethoxysilylpropyl) tetrasulfide (TESPT), was used to modify the surface of multiwalled carbon nanotubes (MWCNTs) in a two‐step method, and the silane‐modified multiwalled carbon nanotubes (s‐MWCNTs) were combined with NR by solvent casting. The s‐MWCNTs with an amorphous layer were visualized by transmission electron microscopy, the functional groups of which were confirmed by Raman and Fourier transform infrared analyses, and the functionalization degree was characterized by thermogravimetric analysis. The interface between s‐MWCNTs and NR was investigated by Raman analysis and field emission scanning electron microscopy (FESEM). Raman analysis showed a shift from 1,340 to 1,353 cm^−1^ of D band of s‐MWCNTs in the NR/s‐MWCNT composite, and FESEM observation indicated that s‐MWCNTs were embedded deeply in NR. All of these results proved that s‐MWCNTs were grafted with TESPT and they reacted with the active double bonds of NR to form a strong interface. The improved interface resulted in an extreme nonlinear viscoelastic behavior and enhanced dynamic mechanical property of NR/s‐MWCNT composite as compared to NR/MWCNT composite. POLYM. COMPOS., 2011. © 2010 Society of Plastics Engineers