Sustainable Benzoxazine Copolymers with Enhanced Thermal Stability, Flame Resistance, and Dielectric Tunability

Benzoxazine resins are gaining attention for their impressive thermal stability, low water uptake, and strong mechanical properties. In this work, two new bio-based benzoxazine monomers were developed using renewable arbutin: one combined with 3-(2-aminoethylamino) propyltrimethoxysilane (AB), and the other with furfurylamine (AF). Both were synthesized using a simple Mannich-type reaction and verified through FT-IR and ¹H-NMR spectroscopy. By blending these monomers in different ratios, copolymers with adjustable thermal, dielectric, and surface characteristics were produced. Thermal analysis showed that the materials had broad processing windows and cured effectively, while thermogravimetric testing confirmed excellent heat resistance-especially in AF-rich blends, which left behind more char. The structural changes obtained during curing process were monitored using FT-IR, and XPS verified the presence of key elements like carbon, oxygen, nitrogen, and silicon. SEM imaging revealed that AB-based materials had smoother surfaces, while AF-based ones were rougher; the copolymers fell in between. Dielectric testing showed that increasing AF content raised both permittivity and loss, and contact angle measurements confirmed that surfaces ranged from water-repellent (AB) to water-attracting (AF). Overall, these biopolymers (AB/AF copolymers) synthesized from arbutin combine environmental sustainability with customizability, making them strong candidates for use in electronics, protective coatings, and flame-resistant composite materials.