Critical temperatures in the synthesis of graphene-like materials by thermal exfoliation–reduction of graphite oxide

We prepared a series of graphene-like materials by thermal exfoliation/reduction of a graphite oxide (GO) at temperatures between 127 °C and 2400 °C. The extent of the exfoliation and reduction of the GO at different temperatures, as well as the impact on the resultant graphene-like materials (TRGs), were studied through their chemical/structural characterization. The main oxygen loss was observed at 127 °C during the blasting of the GO, which produced its exfoliation into monolayer functionalized TRG with hydroxyl groups and minor amounts of epoxy and carboxyl groups. Above 600 °C, the reduction continued smoothly, with oxygen and hydrogen loss and the conversion of hybridised carbon atoms from sp3 into sp2. 1000 °C appears to be a critical temperature for the efficiency of the reduction process, as the resulting TRG contained <2% oxygen and 81.5% sp2-carbon atoms. The materials obtained at 2000 °C and 2400 °C were almost oxygen-free and the layers exhibited a dramatic restoration of the pristine graphite structure, as confirmed by the increase in the average size of the sp2-domains. The typical disordered stacking of TRGs increases with temperature, although they can be dispersed yielding monolayers at 127 and 300 °C and stacks of up to 4–6 layers above 1000 °C, as determined by AFM.