Journal
CATALYSIS LETTERS
Volume 96, Issue 1-2, Pages 13-22Publisher
SPRINGER
DOI: 10.1023/B:CATL.0000029523.22277.e1
Keywords
microkinetic modeling; thermodynamic consistency; rate determining step; most abundant reaction intermediate; adsorbate-adsorbate interactions; density functional theory; ammonia; hydrogen
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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 NH3 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.
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