Chemometric tools were employed to analyze the in-situ dynamic X-ray absorption spectroscopy data to probe the state of Co-MCM-41 catalysts during reduction in pure hydrogen and under single-wall carbon nanotube synthesis reaction conditions. The use of the progressive correlation analysis established the sequence in which changes in the spectral features near the Co K edge occurred. and the evolving factor analysis provided evidence for the formation of an intermediate Co1+ ionic species during reduction of the Co-MCM-41 catalyst in pure hydrogen up to 720 degrees C. This intermediate species preserves the tetrahedral environment in the silica framework and is resistant to complete reduction to the metal in H-2. While the Co2+ species is resistant to reduction in pure CO, the intermediate Co1+ species is more reactive in CO most likely forming cobalt carbonyl-like compounds with high mobility in the MCM-41, These mobile species are the precursors of the metallic clusters growing carbon nanotubes. Controlling the rates of each step of this two-stage reduction process is key to controlling the size of the metallic Co clusters formed in Co-MCM-41 catalysts.