Abstract
Selective catalytic reduction of NO by NH3 over supported vanadium oxide catalysts has been studied for decades, but the studies mostly concentrated on the dominant N2 product with much less attention paid to the formation of the undesired N2O product. In the present study, fundamental aspects of the N2O formation reaction were elucidated by a series of temperature-programmed surface reaction studies with isotopic labelled reactants. The surface vanadium oxide species on the TiO2 support are active sites for the N2O formation reaction, while tungsten species mainly function as promoters. Oxygen from NO, gaseous O2 and catalyst oxygen all function as oxygen sources for formation of N2O (∼50%, ∼30% and ∼20%, respectively). The rate-determining-step for N2O formation involves breaking of the ammonia NH bond. These new molecular level insights have the potential to guide the rational design of improved SCR catalysts for diesel engines with reduced N2O produced.
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