Journal or Book Title
Journal of Chemical Physics
The gas phase reaction of molecular oxygen and hydrogen catalyzed by a Au3cluster to yield H2O2 was investigated theoretically using second order Z-averaged perturbation theory, with the final energies obtained with the fully size extensive completely renormalized CR-CC(2,3) coupled clustertheory. The proposed reaction mechanism is initiated by adsorption and activation of O2 on the Au3cluster. Molecular hydrogen then binds to the Au3O2 global minimum without an energy barrier. The reaction between the activated oxygen and hydrogen molecules proceeds through formation of hydroperoxide (HO2) and a hydrogen atom, which subsequently react to form the product hydrogen peroxide. All reactants, intermediates, and product remain bound to the goldcluster throughout the course of the reaction. The steps in the proposed reaction mechanism have low activation energy barriers below 15kcal∕mol. The overall reaction is highly exothermic by ∼30kcal∕mol.
Copyright 2008 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.
American Institute of Physics
Njegic, Bosiljka and Gordon, Mark S., "Reaction mechanism of the direct gas phase synthesis of H2O2 catalyzed by Au3" (2008). Chemistry Publications. 513.