A sustainable and effective method for de-oxygenation of few-layer graphene oxide (FLGO) by glycerol gasification in supercritical water (SCW) is described. In this manner, reduction of FLGO and valorization of glycerol, in turn catalyzed by FLGO, are achieved simultaneously. The addition of glycerol enhanced FLGO oxygen removal by up to 59% due to the in situ hydrogen generation as compared to the use of SCW only. Physicochemical characterization of the reduced FLGO (rFLGO) showed a high restoration of the sp²-conjugated carbon network. FLGO sheets with a starting C/O ratio of 2.5 are reduced by SCW gasification of glycerol to rFLGO with a C/O ratio of 28.2, above those reported for hydrazine-based methods. Additionally, simultaneous glycerol gasification resulted in the concurrent production of H₂, CO, CH₄ and valuable hydrocarbons such as alkylated and non-alkylated long chain hydrocarbon (C12-C31), polycyclic aromatic hydrocarbons (PAH), and phthalate, phenol, cresol and furan based compounds.
Keywords: few-layer graphene oxide; glycerol gasification; hydrogen production; reduced graphene oxide; supercritical water.