Fabrication and Enhanced Flexibility of Starch-Based Cross-Linked Films

The development of sustainable materials has driven significant interest in starch as a renewable and biodegradable polymer. However, the inherent brittleness, hydrophilicity, and lack of thermoplasticity of native starch limit its application in material science. This study addresses the limitations of native starch by converting it to dialdehyde starch (DAS) and cross-linking with polyether diamines via imine bonds. The effects of Jeffamine molecular weights (D-2000, D-400, and D-230) and mole ratios on the mechanical, thermal, and structural properties of starch-based films were examined. The cross-linked DAS/Js films exhibited significant enhancements in flexibility and toughness. Specifically, DAS/J2000 at a 0.03 mol ratio achieved a tensile strength of 62.9 MPa. In comparison, DAS/J400 at a 0.5 mol ratio demonstrated 126.2% elongation at break, indicating the balance between cross-linking density and chain mobility. X-ray diffraction (XRD) analysis revealed reduced crystallinity and tighter molecular packing with increased cross-linking. Dynamic mechanical analysis (DMA) indicated a decrease in Tg with an increasing mole ratio, reflecting enhanced molecular mobility. The results underscore the potential of optimized cross-linking conditions to produce starch-based films with properties that contribute to developing sustainable biopolymer materials.