The NO/H-2 reaction has been studied over a Ni loaded carbon film catalysts using in situ FTIR spectroscopy at the temperature range 25 -350 degreesC. On these catalysts, the differences in activity and selectivity were found depending on the nature of the surface functional groups. These differences were correlated with transient infrared spectral features which appeared during the reaction. It has been proved experimentally that the chemical character of the support is of vital importance during the process. The rise in NO conversion and N-2 selectivity was observed when the surface of the catalysts was changed by the NH3 chemisorption. Amide and/or imide species formed due to the reduction of ammonium salts of carboxylic acids can play a significant role as active centers during the NO reduction.