The stoichiometry of the low-temperature reaction between surface α-oxygen formed by decomposing N2O over Fe-containing ZSM-5 zeolite and methane, hydrogen (deuterium), and carbon monoxide is studied. Methane and hydrogen react with α-oxygen in stoichiometric ratios of 1 : 1.8 and 1 : 1.6, respectively. The observed stoichiometry is due to the mechanisms of the corresponding reactions. According to a mechanism proposed for the interaction of α-oxygen with methane and hydrogen, this reaction is accompanied by the dissociation of CH4and H2molecules. For hydrogen, such a mechanism is supported by IR spectroscopic studies of resulting surface compounds, namely, of new hydroxyl groups that were formed on the zeolite surface in the course of the reaction. α-Oxygen reacts with CO in the ratio of 1 : 1 to form CO2in amounts equal to those of α-oxygen on the surface.