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Title: Predicting Catalysis: Understanding Ammonia Synthesis from First-Principles Calculations
Authors: Hellman, A. 
Baerends, E. J. 
Biczysko, M. 
Bligaard, T. 
Christensen, C. H. 
Clary, D. C. 
Dahl, S. 
Harrevelt, R. van 
Honkala, K. 
Jonsson, H. 
Kroes, G. J. 
Luppi, M. 
Manthe, U. 
Nørskov, J. K. 
Olsen, R. A. 
Rossmeisl, J. 
Skúlason, E. 
Tautermann, C. S. 
Varandas, A. J. C. 
Vincent, J. K. 
Issue Date: 14-Sep-2006
Publisher: American Chemical Society
Citation: The Journal of Physical Chemistry B. 110:36 (2006) 17719-17735
Abstract: Here, we give a full account of a large collaborative effort toward an atomic-scale understanding of modern industrial ammonia production over ruthenium catalysts. We show that overall rates of ammonia production can be determined by applying various levels of theory (including transition state theory with or without tunneling corrections, and quantum dynamics) to a range of relevant elementary reaction steps, such as N2 dissociation, H2 dissociation, and hydrogenation of the intermediate reactants. A complete kinetic model based on the most relevant elementary steps can be established for any given point along an industrial reactor, and the kinetic results can be integrated over the catalyst bed to determine the industrial reactor yield. We find that, given the present uncertainties, the rate of ammonia production is well-determined directly from our atomic-scale calculations. Furthermore, our studies provide new insight into several related fields, for instance, gas-phase and electrochemical ammonia synthesis. The success of predicting the outcome of a catalytic reaction from first-principles calculations supports our point of view that, in the future, theory will be a fully integrated tool in the search for the next generation of catalysts.
ISSN: 1520-6106
DOI: 10.1021/jp056982h
Rights: openAccess
Appears in Collections:FCTUC Química - Artigos em Revistas Internacionais

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