In situ characterization of interaction of ammonia with carbon surface in oxygen atmosphere

The adsorption and oxidation of ammonia over carbons differing in the chemical structure of surface functional groups have been investigated by FTIR spectroscopy. The reactions of NH3 with carbons have been studied both in the presence and in the absence of oxygen. As a result of NH3 chemisorption, in addition to ammonium salts, there are formed surface amide and imide structures. At the higher temperature surface isocyanate species are formed. Thermal stabilities of surface structures, formed as a result of NH3 chemisorption have been determined by means of FTIR spectroscopy. The activity and selectivity of carbons for the selective catalytic oxidation (SCO) of NH3 to N-2 with excess O-2 has been shown by microreactor studies at 295-623 K. Carbon catalysts are very active for NH3 oxidation. Nitrogen is generally the predominant product of ammonia oxidation. The selectivity to N-2, N2O and NO is determined by the surface oxygen coverage and reaction temperature. The data obtained indicate that the N-2 is formed via selective catalytic reduction (SCR) between NHx surface species and NO formed from NH4+ oxidation. This implies that ammonia is activated in the form of NH4+ species for both SCR and SCO processes. (C) 2003 Elsevier Ltd. All rights reserved.