Automated reaction path search calculations of spin-inversion mechanisms in the 6,4,2Nb + C2H4 reaction

被引：11
作者：
Kawano, Masahiro [1 ]
Koido, Shoichi [1 ]
Nakatomi, Taiki [1 ]
Watabe, Yuya [1 ]
Takayanagi, Toshiyuki [1 ]
机构：
[1] Saitama Univ, Dept Chem, Sakura Ku, Shimo Okubo 255, Saitama, Saitama 3388570, Japan
来源：
COMPUTATIONAL AND THEORETICAL CHEMISTRY | 2019年 / 1155卷
关键词：
Spin-forbidden reaction; Intersystem crossing; Spin-inversion; Transition metal; Reaction mechanism; POTENTIAL-ENERGY SURFACES; TRANSITION-STATE; CHEMICAL-REACTIONS; METAL ATOMS; KINETICS; FORMALDEHYDE; EXPLORATION; ACTIVATION; PREDICTION; COMPLEXES;
D O I：
10.1016/j.comptc.2019.03.021
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
The mechanisms of C-H bond activation in C2H4 by Nb-6,Nb-4,Nb-2 metal atom have been systematically investigated using the automated reaction path search calculation with the mixed-spin Hamiltonian model. It is found that the most stable (NbC2H2)-Nb-4 + H-2 products are formed from the Nb-6 + C2H4 reactants on the sextet, quartet, and double potential energy surfaces via multiple spin-inversion (intersystem crossing) points, which are mostly associated with hydrogen atom transfer. The spin-inversion mechanisms have been further investigated by analyzing the crossing behaviors of the potential energy profiles with different spin multiplicities. We also discuss the importance of multidimensional effects on the spin-inversion dynamics.
引用
收藏
页码：31 / 37
页数：7
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