The detailed mechanisms of carbon monoxide-induced N-N bond cleavage of nitrous oxide (N2O) leading to the nitrosyl isocyanate complex and oxygen atom transfer to carbon monoxide to give metal-bound carbonyl complex have been studied computationally via density functional theory calculations at the B3LYP level.Full free energy profiles are calculated for two different reactions.The calculation results indicate that the two reactions are competitive with each other due to the comparable activation barriers.The metal-bound carbonyl complex obtained from oxygen atom transfer can be recycled to give more nitrosyl isocyanate complexes.In addition,we also demonstrate that the analogous tungsten complex cannot give nitrosyl isocyanate complex via the carbon monoxide-induced N-N bond cleavage of nitrous oxide.The calculations are consistent with experimental observations.