We propose to study a model phyllosilicate catalyst that, upon brief thermal treatment, releases OH groups from its surface to generate pockets of coordinatively unsaturated metal sites in proximity to deprotonated OH groups. This surface structure makes the materials highly effective at performing oxidation and hydrogenation reactions. The proposed experiment will consist of two parts. The first will focus on the in situ activation of the Ni3Si2O5(OH)4 phyllosilicate in order to better understand the structure of the bulk materials. The second phase of the experiment will characterize the ability of the phyllosilicate to activate small molecules. These experiments will generate new knowledge about the mechanism for activating small molecules during catalytic reactions and will greatly assist in the design of new heterogeneous catalysts.