Theoretical Suggestion Of A Methane Hydroxylation Catalyst

Motivated by a recent study on light-induced solar cell that Iridium-oxo complex over WO3 electrode catalyze water oxidation reaction, we investigated the methane hydroxylation reaction by the same complex. Herein we focused on the closed-shell singlet state reaction due to the no-radical intermediate mechanism although this reaction is energetically unfavored reaction. Using intrinsic bond orbital analysis, we found that the C-H bond cleavage reaction proceed via the hydride transfer mechanism. From the view point of orbital interaction between sigma orbital (C-H bond in methane) and pi* orbital (Ir=O bond in Ir complex), we demonstrated that the reactivity of the methane hydroxylation reaction in the closed shell singlet state depends on the energy level of pi* orbital.