原子与分子物理学报Issue(6)：944-961,18.DOI:10.3969/j.issn.1000-0364.2015.12.008
气相钌原子与氮分子作用机理计算研究
Theoretical study on the interaction mechanism of ruthenium atom with nitrogen molecule in gas phase
摘要
Abstract
The geometrical and electronic structures, bonding properties, and vibrational frequencies of complex RuN2 and compound NRuN in linear and bent structures with different multiplicity and electronic states were studied by B3 LYP method using 6-311+G∗and LANL2 DZ basis sets. The transition states for transformation between linear and bent structures and insertion reaction were calculated, and the potential energy curves ob-tained. The results indicate that N2 molecule was activated slightly in most stable electronic states of the comple-xes, 3Δand 3∑- states are more stable than the ground states of the reactants. There were some electrons trans-ferred from Ru atom to N2 molecule viaσ/πdonation and backing. Compared to experiment reported, the struc-ture and vibrational characteristics of compound NRuN in 13 B1 and 11 A1 states are agreed well and proposed as the plausible candidates for the experimental result. Most of electronic states of compound NRuN formed from Ru (a5F) +2N(4S) are exothermic. Ru atom direct insertion into the triple bonds N2 is much more difficult because the energy barriers are higher and the products are thermodynamic instability.关键词
Ru原子/N2 分子/插入反应/势能曲线/密度泛函方法Key words
Ruthenium atom/Nitrogen molecule/Insertion reaction/Potential energy curves/Density function-al theory分类
化学化工引用本文复制引用
王燕妮,金芩,孙晓玲,蔡跃飘,王朝杰..气相钌原子与氮分子作用机理计算研究[J].原子与分子物理学报,2015,(6):944-961,18.基金项目
国家自然科学基金(21177098) （21177098）
温州市科技局项目(Y20080103) （Y20080103）
