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

Abstract

The entire reaction mechanism for the gas-phase CO(C_¥v,¹S⁺) + N₂O(C_¥v,¹S) ® N₂ (D_¥h,¹S⁺_g) + CO₂(D_¥h,¹S_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.