Combined Density Functional Theory and Kinetic Monte Carlo Study of Selective Oxidation of NH3 on Rutile RuO2(110) at Ambient Pressures
Abbreviated Journal Title
J. Phys. Chem. C
HETEROGENEOUS CATALYSIS; AMMONIA; SURFACE; MECHANISM; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, ; Multidisciplinary
We have carried out combined density functional theory (DFT) and kinetic Monte Carlo (KMC) simulations for ammonia oxidation on RuO2(110) using a database of 24 reaction processes (36 processes if reverse processes are counted separately) and compared the selectivity for reaction products under ultrahigh vacuum (UHV) and ambient pressures at selected temperatures. We find that in keeping with earlier experimental and theoretical findings NO selectivity is almost 100% above 600 K in UHV. However, this selectivity disappears for reactions at ambient pressures. We relate the lack of selectivity under ambient pressures to the propensity for NO to convert to N2O and to active recombination of N-cus + N-cus owing to the abundant supply of N species in ambient pressure as a result of active. NHx decomposition by plenty of O species on the RuO2(110) surface.
Journal of Physical Chemistry C
"Combined Density Functional Theory and Kinetic Monte Carlo Study of Selective Oxidation of NH3 on Rutile RuO2(110) at Ambient Pressures" (2014). Faculty Bibliography 2010s. 6073.