Halloysite Nanotubes Reinforced Epoxy/Epoxy Acrylate Blends: Unlocking the Potential of Hybrid Nanocomposites

Unlocking the potential of polymer blends requires innovative strategies that transcend simple mixing. This study presents a novel approach by creating hybrid blends of epoxy and structurally compatible in situ synthesized epoxy acrylate (vinyl ester) resins, further reinforced with halloysite nanotubes (HNTs). We went beyond simple blending by synthesizing the epoxy acrylate (EA) component from the base epoxy resin, ensuring molecular-level compatibility. The epoxy acrylate was successfully synthesized via a ring-opening reaction, as confirmed by FTIR and ¹H-NMR. A series of blends at varying weight ratios of epoxy/epoxy acrylate (75/25, 50/50, and 25/75) was prepared and optimized using dynamic mechanical analysis (DMA) for the best viscoelastic performance and subsequently reinforced with 2 wt% HNTs. Our findings reveal that this unique approach fosters highly interpenetrated polymer networks (IPNs), as evidenced by thermal and viscoelastic behavior. The hybrid epoxy nanocomposite with a 75/25 blend ratio exhibits a superior balance of properties, demonstrating a synergistic enhancement in both thermal and thermomechanical properties compared to the neat epoxy and epoxy acrylate networks. The optimized hybrid epoxy composite exhibits a 147% increase in storage modulus (<i>E</i>') and a 180% increase in loss modulus (<i>E</i>″) over the neat epoxy composite while enhancing thermal stability. This study not only presents HNT-reinforced epoxy/epoxy acrylate as a new family of robust hybrid nanocomposites but also provides a fundamental blueprint for compatibilizing and reinforcing thermoset blends for advanced applications.