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While first-row transition metal cations, notably Fe(+), catalyze the gas-phase conversion of acetylene to benzene, a distinct path is chosen in systems with Os, Ir, and Rh cations. Rather than losing the metal cation M(+) from the benzene–M(+) complex, as is observed for the Fe(+) system, the heavy metal ions activate CH bonds. The landmark system C4H4-Os(+) reacts with acetylene to produce C6H4-Os(+) and dihydrogen. Following our work on isomers of the form C2nH2n-Fe(+), we show by DFT modeling that the CH bonds of the metalla-7-cycle structure, C6H6-Os(+), are activated and define the gas-phase reaction path by which H2 is produced. The landmark structures on the network of reaction paths can be used as a basis for the discussion of reactions in which a single Os atom on an inert surface can assist reactions of hydrocarbons.

CH Activation by a Heavy Metal Cation: Production of H2 from the Reaction of Acetylene with C4H4-Os(+) in Gas phase