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运用密度泛函理论(density functional theory,DFT)方法,在Becke3LYP/Lanl2dz水平下,对团簇CoFe_2B_2各个可能的构型进行优化,最终得到9种优化构型。本文从动力学、热力学稳定性2个方面对这9种构型之间的异构化反应进行分析,发现异构化反应的限度受团簇热力学稳定性的影响,提出一种线性方程lnK=0.391 9ΔE+0.435 7以预测团簇异构化反应的限度;多数构型通过一种或多种通道向构型2~((2))转化;构型1~((4))、2~((4))两者之间的反应为可逆反应,构型1(2)无异构化反应发生并且具有很好的稳定性,最终存在构型为1(2)、2~((2))、1~((4))、2~((4)),即戴“帽”三角锥和四角方锥两类构型。
The density functional theory (DFT) method was used to optimize the possible configurations of CoFe_2B_2 clusters at the Becke3LYP / Lanl2dz level. Finally, nine optimized configurations were obtained. In this paper, the kinetics and thermodynamic stability of these 9 kinds of isomerization reactions were analyzed. It is found that the limit of isomerization reaction is affected by the thermodynamic stability of the clusters. A linear equation lnK = 0.391 9ΔE + 0.435 7 to predict the extent of the cluster isomerization reaction; most configurations were converted to configuration 2 ~ (2) through one or more channels; Configuration 1 ~ (4) The reaction between the two is reversible. The isomerization reaction of configuration 1 (2) takes place with good stability and the final configuration is 1 (2), 2 ~ (2 )), 1 ~ ((4)), 2 ~ (4), that is, wear “hat ” triangular pyramid and square pyramid two kinds of configurations.