Supercritical alcohols as solvents and reducing agents for the synthesis of reduced graphene oxide

We report on a facile, simple, and green graphene oxide (GO) reduction method based on a supercritical alcohol approach. The influence over the chemical, thermal, morphological, and textural properties of reduced graphene oxides (RGOs) of five different alcohols in their supercritical conditions - methanol, ethanol, 1-propanol, 2-propanol, and 1-butanol - was investigated in detail. Although the thermal stabilities and Fourier-transform infrared spectra of RGOs produced using the different alcohols are very similar, a substantial difference in the carbon-to-oxygen ratios measured by X-ray photoelectron spectroscopy and Brunauer-Emmett-Teller surface areas are observed. The RGO produced using supercritical ethanol exhibited a much higher carbon-to-oxygen ratio of 14.4 and a much larger surface area of 203 m²/g compared with that produced using the other supercritical alcohols. Raman spectra showed that the RGOs produced using supercritical ethanol and supercritical 2-propanol retained more of the graphitic structure. X-ray diffraction analysis revealed that RGOs produced using supercritical 1-propanol and supercritical 1-butanol retained at least two different interlayer spacings. The deoxygenation mechanism of GO in supercritical ethanol is proposed based on gas and liquid product analysis.