The potential energy surfaces of N2O2 species: implications for selective catalytic reduction

Abstract

Stationary structures, both minima and transition states, on the potential energy surface of N₂O₂ have been determined using large basis sets and high levels of theory. Minima have been found at the ab initio [BD(T)] and density functional theory (B3LYP) levels, and transition structures have been located at the latter level. These calculations have allowed reaction pathways to the formation of O₂ and N₂ to be explored. A likely initial intermediate is a non-cyclic covalently bound dimer with a barrier to formation sufficiently low to suggest that it might be a candidate for a catalytic mechanism. Subsequent steps towards N₂ and O₂ involve larger barriers, so that substantial catalytic activation would be required for them to be involved in a facile reaction mechanism.