The Role of Intercalated Water in Multilayered Graphene Oxide

A detailed in situ infrared spectroscopy analysis of single layer and multilayered graphene oxide (GO) thin films reveals that the normalized infrared absorption in the carbonyl region is substantially higher in multilayered GO upon mild annealing. These results highlight the fact that the reduction chemistry of multilayered GO is dramatically different from the single layer GO due to the presence of water molecules confined in the ∼1 nm spacing between sheets. IR spectroscopy, XPS analysis, and DFT calculations all confirm that the water molecules play a significant role interacting with basal plane etch holes through passivation, via evolution of CO(2) leading to the formation of ketone and ester carbonyl groups. Displacement of water from intersheet spacing with alcohol significantly changes the chemistry of carbonyl formation with temperature.