The selective catalytic reduction of N2O with CH4 in the presence of excess O-2 (CH4-SCRN2O) and CH4 + O-2 reaction were studied on Ni-MOR, Co-MOR and Fe-MOR, prepared from H-MOR or Na-MOR, by ionexchange or CVD. FTIR showed that transition metal ions (tmi) were well dispersed, mainly isolated with at least two coordinative vacancies. For CH4-SCRN2O, irrespective of Bronsted acid site and Na* amount, catalysts were active in the order Fe-MOR >Ni-MOR > Co-MOR. Using a methane-poor mixture, on all samples CH4-SCRN2O consisted of two nearly independent reactions: CH4 +N2O and CH4+ O-2. Using a methanerich mixture, CH4-SCRN2O consisted of a CH4+ N2O + O-2 reaction, whose stoichiometric ratios depended on the tmi. Whereas on Ni-MOR methane combustion occurred as side reaction, on Co-MOR and Fe-MOR no side reactions occurred. Accordingly, for CH4 + O-2 Co-MOR and Fe-MOR were poorly active, whereas Ni-MOR were highly active. We conclude that in CH4-SCRN2O a monoatomic oxygen form activates methane on Co-MOR and FeMOR catalysts, whereas both a monoatomic oxygen form and a molecular oxygen form activate methane on Ni-MOR. Being active for the CH4-SCRN2O and CH4-SCRNOx and forming CO only in traces, Ni-MOR are promising catalysts for the simultaneous SCR of N2O and NOx using CH4 as reducing agent. (C) 2013 Elsevier B.V. All rights reserved.