Automatic analysis of computed catalytic cycles

Authors

  • Andreas Uhe,

    Corresponding author
    1. Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Worringerweg 1, Aachen 52074, Germany
    • Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Worringerweg 1, Aachen 52074, Germany
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  • Sebastian Kozuch,

    Corresponding author
    1. Institute of Chemistry and the Lise Meitner-Minerva Center for Computational Quantum Chemistry, Hebrew University of Jerusalem, Givat Ram Campus, Jerusalem 91904, Israel
    Current affiliation:
    1. Department of Organic Chemistry, The Weizmann Institute of Science, IL-76100 Rehovot, Israel
    • Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Worringerweg 1, Aachen 52074, Germany
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  • Sason Shaik

    1. Institute of Chemistry and the Lise Meitner-Minerva Center for Computational Quantum Chemistry, Hebrew University of Jerusalem, Givat Ram Campus, Jerusalem 91904, Israel
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Abstract

The energetic span model allows the estimation of the turnover frequency (TOF) of a catalytic reaction from its calculated energy profile. Furthermore, by identifying the TOF determining intermediate and the TOF determining transition state, the model shows that the concept of “determining states” is more useful and correct than the concept of “determining steps.” This article illustrates the application of the model and provides an introduction to its concepts using instructive examples. The first part explains the model in its current state of development, whereas in the second part the degree of TOF control of the reactant and product concentrations is introduced. With this information, it is possible to give explicit recommendations regarding the conditions to be applied in the experiment, e.g., which reactant promotes the reaction or if a product kinetically inhibits it. At the end, we present the AUTOF program that allows the user to apply the complete model in a black box fashion. © 2010 Wiley Periodicals, Inc. J Comput Chem, 2011

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