Abstract
AbstractReported here is the N2cleavage of a one‐electron oxidation reaction usingtrans‐[Mo(depe)2(N2)2] (1) (depe=Et2PCH2CH2PEt2), which is a classical molybdenum(0)‐dinitrogen complex supported by two bidentate phosphine ligands. The molybdenum(IV) terminal nitride complex [Mo(depe)2N][BArf4] (2) (BArf4=B(3,5‐(CF3)2C6H3)4) is synthesized by the one‐electron oxidation of1upon addition of a mild oxidant, [Cp2Fe][BArf4] (Cp=C5H5), and proceeds by N2cleavage from a MoII‐N=N‐MoIIstructure. In addition, the electrochemical oxidation reaction for1also cleaved the N2ligand to give2. The dimeric Mo complex with a bridging N2is detected by in situ resonance Raman and in situ UV‐vis spectroscopies during the electrochemical oxidation reaction for1. Density‐functional theory (DFT) calculations reveal that the unstable monomeric oxidized MoIspecies is converted into2via the dimeric structure involving a zigzag transition state.
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