A facile in situ polymerization was developed for grafting renewable cardanol onto the carbon fiber (CF) surfaces to strengthen the fiber–matrix interface. CFs were chemically modified with hydroxyl groups by using an aryl diazonium reaction, and then copolymerized in situ with hexachlorocyclotriphosphazene (HCCP) and cardanol to build cardanol-modified fibers (CF-cardanol). The cardanol molecules were successfully introduced, as confirmed using Raman spectra and X-ray photoelectron spectroscopy (XPS); the cardanol molecules were found to increase the surface roughness, energy, interfacial wettability, and activity with the matrix resin. As a result, the interlaminar shear strength (ILSS) of CF-cardanol composites increased from 48.2 to 68.13 MPa. In addition, the anti-hydrothermal ageing properties of the modified composites were significantly increased. The reinforcing mechanisms of the fiber–matrix interface were also studied.

In the present research, to enhance interfacial wettability and adhesion between carbon fibers (CFs) and matrix resin, hydrophilic silica nanoparticles (SiO2) were utilized to graft the surface of CFs. Polydopamine (PDA) as a “bio-glue” was architecturally built between SiO2 and CFs to obtain a strong adhesion strength and homogenous SiO2 distribution onto the surface of CFs. The facile modification strategy was designed by self-polymerization of dopamine followed by the hydrolysis of tetraethoxysilane (TEOS) onto carbon fibers. Surface microstructures and interfacial properties of CFs, before and after modification, were systematically investigated. The tight and homogeneous coverage of SiO2 layers onto the CF surface, with the assistance of a PDA layer by self-polymerization of dopamine, significantly enhanced fiber surface roughness and wettability, resulting in an obvious improvement of mechanical interlocking and interfacial interactions between CFs and matrix resin. The interlaminar shear strength (ILSS) and the interfacial shear strength (IFSS) of CF/PDA/SiO2 reinforced composites exhibited 57.28% and 41.84% enhancements compared with those of untreated composites. In addition, impact strength and the hydrothermal aging resistance of the resulting composites showed great improvements after modification. The possible reinforcing mechanisms during the modification process have been discussed. This novel strategy of developed SiO2-modified CFs has interesting potential for interfacial improvements for advanced polymer composites.