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In order to enhance the interfacial adhesion of poly(p-phenylene terephthalamide) (PPTA) fibers to the rubber composites, a novel method to deposit multi-walled carbon nanotubes (MWCNTs) onto the surface of PPTA fibers has been proposed in this study. This chemical modification was performed through the introduction of epoxy groups by Friedel–Crafts alkylation on the PPTA fibers, the carboxylation of MWCNTs, and the ring-opening reaction between the epoxy groups and the carboxyl groups. The morphologies, chemical structures, and compositions of the surface of PPTA fibers were characterized by scanning electron microscope, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The results showed that MWCNTs were uniformly deposited onto the surface of PPTA fibers with the covalent bonds. The measurement of contact angles of the fibers with polar solvent and non-polar solvent indicated that the surface energy of deposited fibers significantly increased by 41.9% compared with the untreated fibers. An electronic tensile tester of single-filament and a universal testing machine were utilized to measure the strength change of the fibers after modification and the interfacial adhesion between the fibers and the rubber matrix, respectively. The results showed that the tensile strength had not been obviously reduced, and the pull-out force and peeling strength of the fibers to the rubber increased by 46.3% and 56.5%, respectively.

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In order to solve the problem of poor interfacial adhesion between aramid fibers and a rubber matrix, an efficient and mild modification method was proposed via polydopamine and mercapto functionalized graphene oxide (GO) and carbon nanotube (CNTs) hybrids synergistically modifying aramid fibers. GO and CNTs were firstly stacked and assembled into unique 3D GO-CNTs hybrids through π-π conjugation. Then, the mercapto functionalization of the assembled 3D GO-CNTs hybrids was realized via the dehydration condensation reaction between the hydroxyls of GO and the silanol groups of coupling agent. Finally, the mercapto functionalized 3D GO-CNTs hybrids were grafted onto the aramid fibers, which were pre-modified by polydopamine through the Michael addition reaction mechanism. The surface morphology and chemical structures of GO-CNTs hybrids and fibers and the interfacial adhesion strength between fibers and rubber matrix were investigated. The results showed that the modification method had brought about great changes in the surface structure of fibers but not generated any damage traces. More importantly, this modification method could improve the interfacial strength by 110.95%, and the reason was not only the reactivity of functional groups but also that the 3D GO-CNTs hybrids with excellent mechanical properties could effectively share interfacial stress. The method proposed in this paper was universal and had the potential to be applied to other high-performance fiber-reinforced composites.