论文标题
天然轨道功能的第二阶 - 底盘（NOF-MP2）方法进行的化学反应性研究。扫描阳离子的水脱氢
Chemical Reactivity Studies by the Natural-Orbital-Functional 2nd-Order-Moller-Plesset (NOF-MP2) method. Water Dehydrogenation by the Scandium Cation
论文作者
论文摘要
最近提出的补充了二阶Møller-plesset计算（NOF-MP2）的自然轨道功能的可靠性，已通过研究通过Scandium Catation研究水的脱氢作用，评估了过渡金属化合物的基本反应的机械研究。高旋转状态势能表面均已彻底搜索。已经特别注意评估NOF-MP2方法的能力，描述了对SC+（3D，1D）对水的反应性的强，静态和动态，电子相关的影响。与实验观察一致，我们的计算正确预测，唯一的放热产物是最低的SCO+（1σ）和H2（1σ_G+）物种。然而，对导致几种其他产品的反应路径进行了深入分析，包括对各种最小值和几个关键过渡态的表征。我们的结果已与高度准确的多材料补充，并补充了准脱位扰动理论，MCQDPT，波函数型计算以及可用的实验数据。据观察，NOF-MP2能够给出令人满意的定量一致性，并且与MCQDPT方法的表现相当。
The reliability of the recently proposed natural orbital functional supplemented with second-order Møller-Plesset calculations, (NOF-MP2), has been assessed for the mechanistic studies of elementary reactions of transition metal compounds by investigating the dehydrogenation of water by the scandium cation. Both high- and low-spin state potential energy surfaces have been searched thoroughly. Special attention has been paid to the assessment of the capability of the NOF-MP2 method to describe the strong, both static and dynamic, electron correlation effects on the reactivity of Sc+(3D,1D) with water. In agreement with experimental observations, our calculations correctly predict that the only exothermic products are the lowest-lying ScO+(1Σ) and H2(1Σ_g+) species. Nevertheless, an in-depth analysis of the reaction paths leading to several additional products was carried out, including the characterization of various minima and several key transition states. Our results have been compared with the highly accurate multiconfigurational supplemented with quasi degenerate perturbation theory, MCQDPT, wavefunction-type calculations, and with the available experimental data. It is observed that NOF-MP2 is able to give a satisfactorily quantitative agreement, with a performance on par with that of the MCQDPT method.
