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Kinetics and dynamics of N2 formation in a steady-state N2O + CO reaction on Pd(110)
Yunsheng Ma1, Song Han, Tatsuo Matsushima
1Catalysis Research Center, Hokkaido University, Sapporo 001-0021 Japan.
Abstract:
The N(2)O decomposition kinetics and the product (N(2) and CO(2)) desorption dynamics were studied in the course of a catalyzed N(2)O+CO reaction on Pd(110) by angle-resolved mass spectroscopy combined with cross-correlation time-of-flight techniques. The reaction proceeded steadily above 400 K, and the kinetics was switched at a critical CO/N(2)O pressure ratio. The ratio was about 0.03 at 450 K and reached approximately 0.08 at higher temperatures. Below it, the reaction was first order in CO, and negative orders above it. Throughout the surveyed conditions, the N(2) desorption sharply collimated along about 45 degrees off the normal toward the [001] direction. Desorbing N(2) showed translational temperatures in the range of 2000-5000 K. It is proposed that the decomposition proceeds in N(2)O(a) oriented along the [001] direction. On the other hand, the CO(2) desorption sharply collimated along the surface normal, showing a translational temperature of about 1600 K.
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