The small metal cluster IrAu+ mediated C–N coupling: A density functional theory study

A detailed investigation of the reaction mechanism underlying the small metal cluster IrAu+ mediated C–N coupling of methane and ammonia has been performed by the density functional theory. At first, both high-spin and low-spin potential energy surfaces are characterized in activation of methane by IrAu+ in detail. Our calculations indicate that the step reaction proceeds on the low-spin potential energy surface although it may involve crossing of potential energy surfaces. The C–H bond of methane could be effectively activated by the cation IrAu+, yielding the bimetallic cation carbene IrAuCH 2 + . Second, the reaction of the product 2 IrAuCH 2 + and ammonia may result in C–N bond coupling, though loss of H 2 ′ in methylene is the most favorable among the three paths dynamically.