Melamine-Functionalized Graphene Oxide as a Multifunctional Modifier for High-Performance Epoxy Nanocomposites with Enhanced Mechanical Properties and Thermal Stability

Developing polymer composites with improved mechanical and thermal properties requires strategies to overcome the problem of agglomeration and weak interfacial interactions of carbon nanofillers. This paper presents an effective strategy for the covalent functionalization of graphene oxide (GO) with melamine to create high-performance epoxy nanocomposites. The functionalization results in the formation of nitrogen-containing heterocyclic structures on the GO surface, as confirmed by FTIR and Raman spectroscopy. The addition of the obtained modified filler (mel-GO) into the epoxy matrix provides a synergistic effect: the melamine amino groups catalytically accelerate curing, reducing the gelation time from 146 to 48 min and increasing the maximum self-heating temperature from 94 to 122 °C, thus indicating enhanced interfacial interaction. This interaction results in a remarkable overall improvement in mechanical properties: tensile and flexural strengths increase by more than 20%, and elastic moduli by 31% and 58%, respectively, compared to the composite containing unmodified GO. At the same time, impact strength (from 14 to 23 kJ/m2) and hardness (up to 87 Shore D) increase. A key achievement is a dramatic increase in thermal and thermal-oxidative stability: the onset temperature of decomposition (T5%) increases by 27 °C, the half-decomposition temperature (T50%) by 45 °C, and the thermal stability index (THRI) increases from 119.3 to 128.9 °C. A more than twofold increase in coke residue yield (to 9.29%) and an increase in the Vicat softening point to 175 °C confirm the formation of an effective thermally stabilizing barrier layer due to the combined action of nitrogen-containing groups and dispersed graphene flakes. The proposed approach to functionalizing graphene oxide with melamine opens the way for the creation of next-generation epoxy composites with a record-breaking combination of strength, impact toughness, and thermal stability for applications in aerospace, electronics, and composite structures operating under extreme conditions.