Title

Combined Density Functional Theory and Kinetic Monte Carlo Study of Selective Oxidation of NH3 on Rutile RuO2(110) at Ambient Pressures

Authors

Authors

S. I. Shah; S. Hong;T. S. Rahman

Comments

Authors: contact us about adding a copy of your work at STARS@ucf.edu

Abbreviated Journal Title

J. Phys. Chem. C

Keywords

HETEROGENEOUS CATALYSIS; AMMONIA; SURFACE; MECHANISM; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, ; Multidisciplinary

Abstract

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 Title

Journal of Physical Chemistry C

Volume

118

Issue/Number

10

Publication Date

1-1-2014

Document Type

Article

Language

English

First Page

5226

Last Page

5238

WOS Identifier

WOS:000333005700019

ISSN

1932-7447

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