Abstract
Mechanistic and kinetic aspects of the direct decomposition of N 2O over steam-activated Fe-silicalite were investigated by transient experiments in vacuum (N 2O peak pressure of ca. 10 Pa) using the temporal analysis of products (TAP) reactor in the temperature range of 773–848 K. The transient responses of N 2O, N 2, and O 2 obtained upon N 2O decomposition were fitted to different micro-kinetic models. Through model discrimination it was concluded that both free iron sites and iron sites with adsorbed mono-atomic oxygen (* O) species are active for N 2O decomposition. Oxygen formation occurs via decomposition of bi-atomic (* O 2) oxygen species adsorbed over the iron site. This bi-atomic oxygen species originates from another bi-atomic oxygen species (O * O), which is initially formed via interaction of N 2O with iron site possessing mono-atomic oxygen species (* O). Based on our modeling, the recombination of two mono-atomic oxygen (* O) species or direct O 2 formation via reaction of N 2O with * O can be excluded as potential reaction pathways yielding gas-phase O 2. The simulation results predict that the overall rate of N 2O decomposition is controlled by regeneration of free iron sites via a multi-step oxygen formation at least below 700 K.
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