Effects of Combining Graphene Nanoplatelet and Phosphorous Flame Retardant as Additives on Mechanical Properties and Flame Retardancy of Epoxy Nanocomposite

The effects of combining 0.1–5 wt % graphene nanoplatelet (GNP) and 3–30 wt % phosphorous flame retardant, 9,10- dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) as fillers in epoxy polymer on the mechanical, flame retardancy, and electrical properties of the epoxy nanocomposites was investigated. GNP was homogeneously dispersed into the epoxy matrix using a solvent-free three-roll milling process, while DOPO was incorporated into the epoxy resin by mechanical stirring at elevated temperature. The incorporation of DOPO reduced the crosslinking density of the epoxy resin. When using polyetheramine as a hardener, the structural rigidity effect of DOPO overshadowed the crosslinking effect and governed the flexural moduli of epoxy/DOPO resins. The flexural moduli of the nanocomposites were improved by adding GNP up to 5 wt % and DOPO up to 30 wt %, whereas the flexural strengths deteriorated when the GNP and DOPO loading were higher than 1 wt % and 10 wt %, respectively. Limited by the adverse effects on mechanical property, the loading combinations of GNP and DOPO within the range of 0–1 wt % and 0–10 wt %, respectively, in epoxy resin were further studied. Flame retardancy index (FRI), which depended on three parameters obtained from cone calorimetry, was considered to evaluate the flame retardancy of the epoxy composites. DOPO showed better performance than GNP as the flame retardant additive, while combining DOPO and GNP could further improve FRI to some extent. With the combination of 0.5 wt % GNP and 10 wt % DOPO, improvement in both mechanical properties and flame retardant efficiency of the nanocomposite was observed. Such a combination did not affect the electrical conductivity of the nanocomposites since the percolation threshold was at 1.6 wt % GNP. Our results enhance the understanding of the structure–property relationship of additive-filled epoxy resin composites and serve as a property constraining guidance for the composite manufacturing.