Effect of long-term ageing on graphene oxide: structure and thermal decomposition

After long-term ageing, the structure of graphene oxide prepared by the modified Hummers method changed. Because of the desorption of oxygen-containing functional groups, the C/O ratio of graphene oxide increased from 1.96 to 2.76. However, the average interlayer distance decreased from 0.660 to 0.567 nm. The content of -CH- and -CH₂- decreased; however, the type of oxygen-containing functional groups did not change. Moreover, I _D/I _G increased from 0.87 to 0.92, indicating that the defect density decreased because of desorbing oxygen functional groups after ageing. When the temperature exceeded 60°C, CO₂ produced by decomposing graphene oxide was detected. The thermal decomposition changed after ageing. The decomposition peak temperature decreased from 216°C to 195°C. The CO₂ amount produced remained almost unchanged; however, the amount of CO, SO₂ and H₂O decreased. After ageing, the apparent activation energy of graphene oxide decreased from 150 to 134 kJ mol^-1.