Full cycle, molecular approach

Platinum and palladium were among the first metals that were investigated in the molecular surface chemistry approach employing free mass-selected metal clusters [159]. The clusters were generated with a laser vaporization source and reacted in a pulsed fast flow reactor [18] or were prepared by a cold cathode discharge and reacted in the flowing afterglow reactor [404] under low-pressure multicollision reaction conditions. These early measurements include the detection of reaction products and the determination of reaction rates for CO adsorption and oxidation reactions. Later, anion photoelectron spectroscopic data of cluster carbonyls became available [405, 406] and vibrational spectroscopy of metal carbonyls in matrices was extensively performed [407]. Finally, only recently, the full catalytic cycles for the CO oxidation reaction with N2O and O2 on free clusters of Pt and Pd were discovered and analyzed [7,408]. 

A DFT quantum mechanical approach is used here to first obtain potential energy profiles along the pseudo-rotational cycle of these model structures. To complete these studies so as to take into account temperature effects (populations), molecular dynamics are investigated in order to study the conformational equilibria. Uncommonly, full quantum... 

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