The synergistic effect of combining different modification methods was investigated in this study to improve the interlaminar toughness and delamination resistance of fiber reinforced polymers (FRP). Epoxy-compatible polysulfone (PSU) was end-capped with epoxide group through functionalization, and the fiber surface was chemically grafted with amino functional group to form a micron-size rough surface. Consequently, the long chain of PSU entangles into crosslinked thermoset epoxy network, additionally, epoxide group on PSU further improves the bonding through chemical connection to the epoxy network and amino group on fiber surface. The combined modification methods can generate both strong physical and chemical bonding. The feasibility of using this method in vacuum assisted resin transfer molding was determined by rheometer. The impact of formed chemical bonds on the crosslinking density was examined through glass transition temperatures. The chemical modifications were characterized by Raman Spectroscopy to determine the chemical structures. Synergistic effect of the modification was established by Mode I and Mode II fracture tests which quantify the improvement on composites delamination resistance and toughness. The mechanism of synergy was explained based on the fracture mode and interaction between the modification methods. Finally, Numerical simulation was used to compare samples with and without modifications. The experiment results showed that synergy is achieved at low concentration of modified PSU because the formed chemical bonds compensate the effect of low crosslinking density and interact with the modified fiber.

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