Reported here is the N 2 cleavage of ao ne-electron oxidation reaction using trans-[Mo(depe) 2 (N 2 ) 2 ]( 1)( depe = Et 2 PCH 2 CH 2 PEt 2 ), which is ac lassical molybdenum(0)-dinitrogen complex supported by two bidentate phosphine ligands. The molybdenum(IV) terminal nitride complex [Mo-(depe) 2 N][BArf 4 ]( 2)( BArf 4 = B(3,5-(CF 3 ) 2 C 6 H 3 ) 4 )i ss ynthesized by the one-electron oxidation of 1 upon addition of amild oxidant, [Cp 2 Fe][BArf 4 ](Cp = C 5 H 5 ), and proceeds by N 2 cleavage from aM o II -N=N-Mo II structure.I naddition, the electrochemical oxidation reaction for 1 also cleaved the N 2 ligand to give 2.The dimeric Mo complex with abridging N 2 is detected by in situ resonance Raman and in situ UV-vis spectroscopies during the electrochemical oxidation reaction for 1.Density-functional theory (DFT) calculations reveal that the unstable monomeric oxidized Mo I species is converted into 2 via the dimeric structure involving az igzag transition state.