Combining Siloxane-Based polybenzoxazine with Poly(ethylene-co-vinyl acetate/hydroxyl) for tougher, more Stable, and Self-Healable materials

Cross-linked EVOH containing dynamic silyl ether bonds with improved toughness and processability have been prepared by taking advantage of both ethylene vinyl alcohol (EVOH) and benzoxazine chemistry. For that, the cross-linked EVOH was synthesized through a trans etherification reaction between siloxane mono-functional benzoxazine and pendant hydroxyl groups on ethylene vinyl alcohol (EVOH) copolymer. The precursor EVOH copolymer was obtained by hydrolysis of the commercially available and inexpensive ethylene–vinyl acetate copolymer (EVA). The chemical structures of polymers were analyzed by proton nuclear magnetic resonance (¹H NMR) spectra and Fourier transform infrared (FTIR) spectroscopy. The curing and thermal stability were researched by using differential scanning calorimetry (DSC) and a thermogravimetric analyzer (TGA), respectively. The mechanical properties via the stress–strain analysis were examined to identify the effect of the benzoxazines with the silyl ether group on the toughness and self-healing ability of the modified EVOH.