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用量子化学密度泛函方法详细研究了双原子铜阴离子Cu-2催化CO氧化形成CO2反应在气相中机理.在UB3LYP结合混合基组水平上,优化了所有反应物,中间体,过渡态和产物的几何构型,并进行了振动分析和波函数稳定性测试.计算结果表明最可能反应通道为CO和O2共吸附到Cu-2,然后形成四元环中间体,最后四元环中间体分解形成产物或另一分子CO进攻四元环中间体从而形成产物.第二个CO分子的协同作用比较小,能垒仅相差0.02eV.最难进行的反应通道为CO从Cu2O-2摘取氧原子形成CO2.Cu-2催化CO氧化反应活性比Au-2好.
Quantum chemical density functional method was used to investigate the mechanism of CO oxidation to CO 2 reaction in the gas phase catalyzed by Cu-2, a Cu atom of diatomic copper. All the reactants, intermediates, transition states and products were optimized at the level of UB3LYP combined with mixed basis set And the vibrational analysis and the stability test of the wave function are carried out.The results show that the most likely reaction channel is the co-adsorption of CO and O2 to Cu-2, then the formation of a four-membered ring intermediate, and the decomposition of the four-membered ring intermediate The formation of the product or another molecule CO offensive four-membered ring intermediates to form the product.The second CO molecules synergistic effect is relatively small, the energy barrier is only 0.02eV difference.The most difficult reaction channel for the removal of CO from Cu2O-2 oxygen Atoms to form CO2. Cu-2 catalytic CO oxidation reaction activity better than Au-2.