Synergism and multiple mechanical relaxations observed in ternary systems based on benzoxazine, epoxy, and phenolic resins

The synergism in the glass-transition temperature (Tg) of ternary systems based on benzoxazine (B), epoxy (E), and phenolic (P) resins is reported. The systems show the maximum Tg up to about 180 °C in BEP541 (B/E/P = 5/4/1). Adding a small fraction of phenolic resin enhances the crosslink density and, therefore, the Tg in the copolymers of benzoxazine and epoxy resins. To obtain the ultimate Tg in the ternary systems, 6–10 wt % phenolic resin is needed. The molecular rigidity from benzoxazine and the improved crosslink density from epoxy contribute to the synergistic behavior. The mechanical relaxation spectra of the fully cured ternary systems in a temperature range of −140 to 350 °C show four types of relaxation transitions: γ transition at −80 to −60 °C, β transition at 60–80 °C, α1 transition at 135–190 °C, and α2 transition at 290–300 °C. The partially cured specimens show an additional loss peak that is frequency-independent as a result of the further curing process of the materials. The ternary systems have a potential use as electronic packaging molding compounds as well as other highly filled systems.