The role of adsorbate-adsorbate interactions in the rate controlling step and the most abundant reaction intermediate of NH3 decomposition on Ru Academic Article

abstract

• N-N adsorbate-adsorbate interactions on a Ru(0001) surface are first estimated using quantum mechanical density functional theory (DFT) calculations, and subsequently incorporated, for the first time, in a detailed microkinetic model for NH 3 decomposition on Ru using the unity bond index-quadratic exponential potential (UBI-QEP) method. DFT simulations indicate that the cross N-H interactions are relatively small. Microkinetic model predictions are compared to ultra-high vacuum temperature programmed desorption and atmospheric fixed bed reactor data. The microkinetic model with N-N interactions captures the experimental features quantitatively. It is shown that the N-N interactions significantly alter the rate determining step, the most abundant reaction intermediate, and the maximum N*-coverage, compared to mechanisms that ignore adsorbate-adsorbate interactions.

authors

• Barteau, Mark

published proceedings

• CATALYSIS LETTERS

author list (cited authors)

• Mhadeshwar, A. B., Kitchin, J. R., Barteau, M. A., & Vlachos, D. G.

citation count

• 66

complete list of authors

• Mhadeshwar, AB||Kitchin, JR||Barteau, MA||Vlachos, DG

publication date

• July 2004

publisher

• Springer Nature  Publisher

published in

• Catalysis Letters  Journal

keywords

• Adsorbate-adsorbate Interactions
• Ammonia
• Density Functional Theory
• Hydrogen
• Microkinetic Modeling
• Most Abundant Reaction Intermediate
• Rate Determining Step
• Thermodynamic Consistency

Digital Object Identifier (DOI)

• 10.1023/B:CATL.0000029523.22277.e1

start page

• 13

end page

• 22

volume

• 96

issue

• 1-2

URL

• http://dx.doi.org/10.1023/b:catl.0000029523.22277.e1