Effects of gaseous environments on physicochemical properties of thermally exfoliated graphene oxides for hydrogen storage: a comparative study

Abstract The present study compared the effect of different gaseous environments on physicochemical properties and subsequent hydrogen storage ability of thermally exfoliated graphene oxide (EGO). The reducing, inert or oxidizing environments were generated using hydrogen, argon or air as the carrier gas, respectively. The structure of thermally exfoliated graphene oxide depended on the type of gaseous environment. The EGO prepared in presence of Air showed the fluffiest layered structure having highest surface area. The surface area order was EGO(Air) (268 m²/g) > EGO(H₂) (248 m²/g) > EGO(Ar) (155 m²/g). The average pore sizes of EGO(Air) and EGO(H₂) were 2.9 and 2.8 nm, with pore volumes of 1.2 and 1.6 cm³/g, respectively. The average pore size for EGO(Ar) was highest at 4.1 nm, associated with presence of larger void space and lowest total pore volume of 1.0 cm³/g. Thus, presence of oxidative or reducing atmosphere seemed to be more conducive to exfoliation of layers by gradual removal of functional groups. The inert atmosphere of argon caused severe thermal separation of layers and functional groups, adversely affecting the layered structure as observed. The EGO(Air) also showed highest O/C ratio suggesting presence of significant amount of oxygen–containing functional groups on the surface. The hydrogen uptake order at 77 K and 30 bar was: EGO (Air) 3.34 wt.% > EGO (H₂) 3.12 wt.% > EGO (Ar) 2.2 wt.%. The highest uptake of EGO(Air) might have resulted from highest surface area, highest O/C ratio and presence of considerable pore volume.