Computer-Guided Development of Hyperbranched Modified Starch-Based Adhesives

In this study, a novel starch-based adhesive (SBA) was proposed, which mainly involved the synthesis of a carboxyl-terminated hyperbranched polymer using bisphenol A diglycidyl ether (DGEBA) and citric acid as raw materials. Subsequently, starch was modified through hyperbranching to enhance the shear strength and water resistance of the SBA. For this purpose, the feasibility of the reaction between DGEBA and citric acid was analyzed using quantum mechanical simulations. Subsequently, both substances were simulated to synthesize carboxyl-terminated hyperbranched polymers with different ratios. Starch was modified through hyperbranching to establish various models of SBAs, and their properties were estimated using molecular dynamics simulations. Theoretical analysis indicates that a DGEBA-to-citric acid ratio of 3:7 yields a SBA with relatively optimal properties. The solubility parameter of this adhesive is 19.05 (J/cm³)¹/², suggesting strong intermolecular interactions between the hyperbranched polymer and starch. The synthesized adhesive exhibits high cohesive strength, with an estimated water contact angle of up to 138°, indicating good hydrophobicity. Furthermore, the system demonstrates favorable mechanical performance, with a shear modulus of 4.34 GPa and a bulk modulus of 8.80 GPa. Additionally, at this ratio, the SBA exhibits a relatively high interaction energy of -408.01 kcal/mol with the cellulose substrate, suggesting that the adhesive possesses favorable shear strength.