To enhance the interfacial adhesion between poly(p-phenylene terephthalamide) (PPTA) fibers and a rubber matrix without damaging the fiber structures, aminated carbon nanotubes (NH₂-CNTs) were mildly deposited onto the fiber surface by combining the biomimetic modification of dopamine via the Michael addition reaction. Furthermore, differences between the “one-step” method and the “two-step” method were researched through adjusting the addition sequence of NH₂-CNTs. The surface morphologies and chemical structures of PPTA fibers before and after modification were characterized by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The mechanical properties of fibers and the adhesive properties with rubber were tested using an electronic tensile tester of single-filament and universal testing machine, respectively. After modification by the “one-step” method for 24 h, the single-filament tensile strength of the modified fibers increased by 16.5%, meanwhile, the pull-out force of the modified fibers to rubber increased by approximately 59.7%. Compared with the “two-step” method, the “one-step” method had superiority due to the short reaction time and the large deposition rate of CNTs.

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.