Simultaneous improvement in the flame resistance and thermal conductivity of epoxy/Al₂O₃ composites by incorporating polymeric flame retardant-functionalized graphene

Fire hazards related to polymer-based thermally conductive composites (PTCs) used in electronic equipment are a significant, but often neglected, risk. Here, we offer a solution by incorporating flame retardant-functionalized graphene (PFR-fRGO) into PTCs using a procedure that improves both their flame resistance and thermal conductivity. Briefly, PFR-fRGO was prepared by covalently grafting a polyphosphoramide oligomer (PDMPD) onto the surface of graphene, which was then introduced in situ into epoxy resin/Al₂O₃ (EP/Al₂O₃) composites. As expected, the incorporation of PFR-fRGO not only increased the thermal conduction paths by weakening the settlement of microparticles, but also reduced the interfacial thermal resistance by enhancing interfacial interactions, both of which resulted in an enhancement of the thermal conductivity of the ternary composites. The resultant EP/Al₂O₃/PFR-fRGO composite exhibited a superior flame retarding ability with dramatic decreases being seen in the high peak heat release rate (PHRR), the total heat release (THR) and the total smoke production (TSP), i.e. 53%, 37% and 57%, respectively, when compared to pure epoxy resin. Additionally, a synergistic flame retarding effect was found in the ternary composite compared to the EP/PFR-fRGO and EP/Al₂O₃ composites. The remarkable enhancement in flame retardancy was mainly attributed to the catalytic charring effect of PFR-fRGO and the template effect of Al₂O₃, both of which resulted in the formation of a high strength, thermally stable protective layer in the condensed phase that is able to retard the permeation of heat and volatile degradation products during combustion, slow down the heat release rate and protect the underlying polymer.