Heterogeneous catalysis first-principles thermodynamic

First-principles Thermodynamic Models in Heterogeneous Catalysis... 

First-principles Thermodynamic Models in Heterogeneous Catalysis The total energy change from initial state <7 to final state [Pg.105]

Rate constants can be estimated by means of transition-state theory. In principle all thermodynamic data can be deduced from the partion function. The molecular data necessary for the calculation of the partion function can be either obtained from quantum mechanical calculations or spectroscopic data. Many of those data can be found in tables (e.g. JANAF). A very powerful tool to study the kinetics of reactions in heterogeneous catalysis is the dynamic Monte-Carlo approach (DMC), sometimes called kinetic Monte-Carlo (KMC). Starting from a paper by Ziff et al. [16], several investigations were executed by this method. Lombardo and Bell [17] review many of these simulations. The solution of the problem of the relation between a Monte-Carlo step and real time has been advanced considerably by Jansen [18,19] and Lukkien et al. [20] (see also Jansen and Lukkien [21]). First principle quantum chemical methods have advanced to the stage where they can now offer quantitative predictions of structure and energetics for adsorbates on surfaces. Cluster and periodic density functional quantum chemical methods are used to analyze chemisorption and catalytic surface reactivity [see e.g. 24,25]. 

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