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State Key Laboratory of Structural Chemistry, Fuzhou, Fujian 350002, China The adsorption and decomposition of N 2O at regular and defect sites of MgO (001) surface have been studied using cluster models embedded in a large array of point charges (PCs) by DFT/B3LYP method. The results indicate that the MgO (001) surface with oxygen vacancies exhibits high catalytic reactivity toward N 2O adsorptive-decomposition. It is different from the regular MgO surface or the surface with magnesium vacancies. Much elongation of O-N bond of N 2O after adsorption at oxygen vacancy site with O end down shows that O-N bond has been broken with concurrent production of N 2, leaving a regular site instead of the original oxygen vacancy site (F center). The MgO (001) surface with magnesium vacancies hardly exhibits catalytic reactivity. It can be concluded that N 2O dissociation likely occurs at oxygen vacancy sites of MgO (001) surface, which is consistent with the generally accepted viewpoint in the experiments. The potential energy surface (PES) reflects that the dissociation process of N 2O does not virtually need to surmount a given energy barrier.
State Key Laboratory of Structural Chemistry, Fuzhou, Fujian 350002, China The adsorption and decomposition of N 2O at regular and defect sites of MgO (001) surface have been studied using cluster models embedded in a large array of point charges (PCs) by DFT / B3LYP method. The results indicate that the MgO (001) surface with oxygen vacancies exhibits high catalytic reactivity toward N 2O adsorptive-decomposition. It is different from the regular MgO surface or the surface with magnesium vacancies. 2O after adsorption at oxygen vacancy site with O end down shows that ON bond has been broken with concurrent production of N 2, leaving a regular site instead of the original oxygen vacancy site (F center). The MgO (001) surface with magnesium vacancies It has been suggested that oxygen vacancy sites of MgO (001) surface, which is consistent with the generally accepted viewpoint i n the experiments. The potential energy surface (PES) reflects that the dissociation process of N 2O does not virtually need to surmount a given energy barrier.