Quantum mechanical models in catalysis



We applied general quantum mechanical ideas in order to establish the form of the many-electron wave functions suitable for analysis of catalytic processes. This led us to the conclusion that the relevant wave functions for the electrons of the catalytic complexes must be taken as superpositions of the antisymmetrized products of the wave functions of electrons in excited and ionized states of the catalyst and reactants. With use of the trial wave function for the electrons of the catalytic complex in such a form, it becomes possible to construct model potential energy surfaces of catalytic reactions as a superposition of the potential energy surfaces of the reactants in different electronic states. We formulate the criteria which when satisfied make it possible to implement a catalytic version of a desired chemical transformation. We also propose an approach to the explanation of the frequently observed correlations between the catalytic activity and other physical properties of a catalyst. © 1996 John Wiley & Sons, Inc.