Toughening and Enhancing Melamine-Urea-Formaldehyde Resin Properties via in situ Polymerization of Dialdehyde Starch and Microphase Separation

The goal of this study is to employ bio-based dialdehyde starch (DAS), derived from in situ polymerization and the resultant microphase separation structure, to improve the strength of melamine-urea-formaldehyde (MUF) resin, as well as enhance the properties that affect its adhesive performance. Thus, we evaluated the effects of DAS on the chemical structure, toughness, curing behavior, thermal stability, and micromorphology of the MUF resin. Furthermore, the wet shear strength and formaldehyde emissions of a manufactured, three-layer plywood were also measured. Results indicate that DAS was chemically introduced into the MUF resin by in situ polymerization between the aldehyde group in the DAS and the amino group and hydroxymethyl group in the resin. Essentially, polymerization caused a DAS soft segment to interpenetrate into the rigid MUF resin cross-linked network, and subsequently form a microphase separation structure. By incorporating 3% DAS into the MUF resin, the elongation at break of impregnated paper increased 48.12%, and the wet shear strength of the plywood increased 23.08%. These improvements were possibly due to one or a combination of the following: (1) DAS polymerization increasing the cross-linking density of the cured system; (2) DAS modification accelerating the curing of the MUF resin; and /or (3) the microphase separation structure, induced by DAS polymerization, improving the cured resin's strength. All the results in this study suggest that the bio-based derivative from in situ polymerization and microphase separation can effectively toughen and enhance the properties that affect adhesive performance in highly cross-linked thermosetting resins.