Melamine formaldehyde resin adhesive toughened with graphene oxide: Structures and properties

The melamine-formaldehyde (MF) resin adhesive was modified by graphene oxide (GO), the chemical structure, wettability, bonding performance, tensile properties, curing performance and thermal properties of the modified resin were analyzed, and the toughening mechanism was also discussed in this study. The results showed that: (1) The MF resin with a high molar ratio possessed stable methylene ether bonds, which could easily generate parallel folding in space to form a π-π stacking supramolecular self-assembly special structure, with the potential of enhancing the toughness of molecular structures. (2) GO contained a large number of oxygen-containing reactive functional groups, which could further lower the curing temperature of the MF resin. A dense cross-linked network structure improved the thermal stability of the resin. (3) The bonding strength and toughness of the resin were significantly improved when the content of GO was 0.1 wt%. However, due to the large specific surface area and the intense π-π interaction between sheets, GO was easy to agglomerate, and the properties of the resin with GO content of 0.4 wt% degraded sharply. (4) The crystallinity of the MF resin modified by GO decreased, and the surface energy and plastic deformation energy increased due to the increased fracture crack path and fracture surface of the resin, which was the macro-reason for the improvement of toughness. (5) The strong π-π interaction between GO sheets and π-π accumulation between triazine rings were like parallel “springs” in the molecular structure of the resin, which might be the internal reason for the improvement of toughness. In addition, it was also proved that this special structure could limit the activity of hydroxymethyl and the release of free formaldehyde in the resin.