Reduction of N2O by H2 catalyzed by platinum monocation: A theoretical study

The Pt+-catalyzed reduction of N2O by H-2 has been theoretically elucidated. The calculated potential energy surfaces indicates that the reactions on doublet surface are both kinetically and thermochemically barrierless, whereas the reactions on quartet Surface are thermochemically favorable, but kinetically unfavorable. The doublet ground state Pt+ cation can be efficient catalyst even under room temperature condition, which agrees well with the experimental observations. The identified reaction mechanisms and the potential energy surfaces indicate that the crossings between the doublet and quartet surfaces are very unlikely to occur. (C) 2009 Elsevier B.V. All rights reserved.