Interactions between CO2 and clay have attracted interest in the scientific community recently. This is partly motivated by the presence of large amounts of clays in caprock formations acting as flow barriers in storage sites for CO2. However, thesorption mechanisms of CO2 by clays are not completely understood, and previous investigations are far from being complete and their results remain controversial. One of the hypotheses for the driving mechanisms is the interaction between the gas and the residual H2O in the clay interlayer space. This interaction would affect (and maybe control) the kinetics of CO2 intercalation. Because of the large incoherent cross section of the hydrogen atom, we will monitor if changes occur in the vibrational spectra and characterize the effects of any interaction that may occur between the gas and the interlayer water in Li- and Ni-fluorohectorite.