【摘要】 对铂原子采用LANl2DZ相对论有效核势基组,对非金属原子采用6-311+G(d)基组,运用密度泛函理论B3LYP方法研究了Pt2O+催化N2O+CO→N2+CO2反应的反应机理.对反应物、中间体、过渡态以及反应产物进行了全结构优化.通过振动频率分析考察了优化的结构是能量极小点还是一级鞍点.采用内禀反应坐标计算验证了所有过渡态连接的相关中间体.结果表明Pt2O+催化反应N2O+CO→N2+CO2(一步反应)是最容易发生的.另一方面,对于反应N2O+CO→N2+CO2,Pt2O+的催化活性比PtO+高.更多还原

【Abstract】 The mechanism for the reaction N2O+CO→N2+CO2 catalyzed by Pt2O+is explored and investigated in terms of density functional theory(DFT(B3LYP)) with the relativistic effective core potential(RECP) of LANl2dz on platinum and 6-311+G(d) basis set on nonmetal atoms.The geometries for reactants,intermediates,transition states,and the products are completely optimized.All the transition states are confirmed by the vibrational frequency analysis and the intrinsic reaction coordinate calculations.The results demonstrate that the reaction N2O+CO→N2+CO2 catalyzed by Pt2O+(a one-step reaction) is most easy to occur.On the other hand,for reaction N2O+CO→N2+CO2,the catalytic activity of Pt2O+is higher than that of PtO+.更多还原