Theoretical Study of Catalytic Reaction Mechanism of CO with N2O by Cu+

The entire reaction mechanism for the gas-phase CO(C-ccv,(1)Sigma(+)) + N2O(C-ccv,(1)Sigma)-> N-2 (D-cch,(1)Sigma(+)(g)) + CO2(D-cch,(1)Sigma(+)(g)) catalytic reaction by the bare Cu+ are discussed by the density function theory(DFT). The calculated results explicitly indicated that the reaction exist spin-forbidden phenomenon between the singlet and the triplet potential energy surfaces (PESs). Two crossing points (CP1 and CP2) which play a significant role in this catalytic reaction. The values of the spin-orbit coupling constants are 673.1 cm(-1) at CP1 and 284.2 cm(-1) at CP2, which indicate that the spin crossing process can occur efficiently due to the large spin-orbit coupling involved. This process made the value of activation energy reduce 108.5 kJ/mol, which are helpful for the reaction on kinetics and thermodynamics.