Toughening of epoxy resins by hydroxy-terminated, silicon-modified polyurethane oligomers

Epoxy resins are among the most versatile engineering structural materials. A wide variety of epoxy resins are commercially available, but most are brittle. Several approaches have been used to improve the toughness of epoxy resins, including the addition of fillers, rubber particles, thermoplastics, and their hybrids, as well as interpenetrating polymer networks (IPNs) of acrylic, polyurethane, and flexibilizers such as polyols. This last approach has not received much attention; none of them have been able to suitably increase resin toughness with out sacrificing tensile properties. Therefore, in an attempt to fill this gap, we experimented with newly synthesized hydroxy-terminated silicon-modified polyurethane (SiMPU) oligomers as toughening agents for epoxy resins. SiMPU oligomers were synthesized from dimethyl dichlorosilane, poly(ethylene glycol) (weight-average molecular weight ∼ 200), and toluene 2,4-diisocyanate and characterized with IR, 1H-NMR and 13C-NMR, and gel permeation chromatography. The synthesized SiMPU oligomers, with different concentrations, formed IPNs within the epoxy resins (diglycidyl ether of bisphenol A). The resultant IPN products were cured with diaminodiphenyl sulfone, diaminodiphenyl ether, and a Ciba-Geigy hardener under various curing conditions. Various mechanical properties, including the lap-shear, peel, and impact strength, were evaluated. The results showed that 15 phr SiMPU led to better impact strength of epoxy resins than the others without the deterioration of the tensile properties. The impact strength increased continuously and reached a maximum value (five times greater than that of the virgin resin) at a critical modifier concentration (20 phr). The critical stress intensity factor reached 3.0 MPa m1/2 (it was only 0.95 MPa m1/2 for the virgin resin).