Simultaneous reduction and functionalization of graphene oxide via antioxidant for highly aging resistant and thermal conductive elastomer composites

Preparation of elastomer/graphene composites with high aging resistance and thermal conductivity is of great significance for constructing many advanced materials, such as solar cells and light emitting diodes. Herein, an efficient one-step approach was developed to simultaneously reduce and functionalize GO via N-1,3-dimethylbutyl-N′-phenyl-p-phenylenediamine (antioxidant 4020). It was found that oxygen-containing groups in GO were effectively removed and sp2 carbon network was restored after reduction. In addition, antioxidant molecules (∼10 wt%) were chemically immobilized on the surface of reduced GO (G-4020). The immobilized antioxidant not only showed much better antimigratory efficiency than free antioxidant in styrene-butadiene rubber (SBR), but also prevented the restacking of G-4020. Consequently, apart from the enhanced mechanical strength, SBR/G-4020 composites exhibited exceptionally high long-term thermo-oxidative aging resistance compared with SBR/r-GO/4020 composites (SBR with hydrazine hydrate reduced GO and 4020). Moreover, the thermal conductivity of SBR/G-4020 composites was superior to that of SBR/r-GO/4020 composites due to the reduced interfacial thermal resistance. Potentially, one-step reaction and high-efficiency make the approach of using antioxidants a promising strategy for the eco-friendly reduction and functionalization of GO, which may offer a new path to construct high-performance elastomer/graphene composites.