Synthesis of conducting graphene/Si3N4 composites by spark plasma sintering

Graphene/silicon nitride (Si3N4) composites with high fraction of few layered graphene are synthesized by an in situ reduction of graphene oxide (GO) during spark plasma sintering (SPS) of the GO/Si3N4 composites. The adequate intermixing of the GO layers and the ceramic powders is achieved in alcohol under sonication followed by blade mixing. The reduction of GO occurs together with the composite densification in SPS, thus avoiding the implementation of additional reduction steps. The materials are studied by X-ray photoelectron and micro-Raman spectroscopy, revealing a high level of recovery of graphene-like domains. The SPS graphene/Si3N4 composites exhibit relatively large electrical conductivity values caused by the presence of reduced graphene oxide (∼1 S cm−1 for ∼4 vol.%, and ∼7 S cm−1 for 7 vol.% of reduced-GO). This single-step process also prevents the formation of highly curved graphene sheets during the thermal treatment as the sheets are homogeneously embedded in the ceramic matrix. The uniform distribution of the reduced GO sheets in the composites also produces a noticeable grain refinement of the silicon nitride matrix.