摘要
根据拓扑学原理从密度泛函理论方面对团簇Fe4P进行全参数优化和频率计算,得到8种优化构型,其中构型1(2)能量最低,稳定性最好,构型5(4)的能量最高,最不稳定。团簇重态的变化对构型稳定性有较大的影响,二重态的各优化构型稳定性好于四重态。综合键级和键长的分析得出Fe1-P和Fe2-P键是团簇Fe4P各优化构型稳定性的主要贡献者,Fe1-Fe2和Fe3-P键对构型作用效果的不同,造成二重态与四重态稳定性存在差异。Fe、P原子对前线轨道HOMO、LUMO均有贡献,其中Fe原子是前线轨道的主要贡献者,说明Fe原子极有可能是团簇Fe4P潜在的催化活性位点。
According to the topological principle,eight optimized configurations were obtained by optimizing all parameters and calculating frequencies using the density functional theory.Among them,configuration 1(2)has the lowest energy and the best stability,and configuration 5(4)has the highest energy and the worst stability.The change in the cluster weight state has a great influence on the stability.The stability of the optimized configurations of the double state is better than that of the quadruple state.The analysis on bond order and bond length shows that Fe1-P and Fe2-P bonds are the main contributors to the stability of the optimized configurations of the Fe4P clusters.The difference in the effect of Fe1-Fe2 and Fe3-P bonds on the configurations results in the stability difference of the two states.Both Fe and P atoms contribute to the front-line orbital HOMO and LUMO,while Fe atom is the main contributor,indicating that Fe atom is very likely to be the potential catalytic active site of the Fe4P cluster.
作者
侯欠欠
方志刚
秦渝
HOU Qianqian;FANG Zhigang;QIN Yu(School of Chemical Engineering,University of Science and Technology Liaoning,Anshan 114501,China)
出处
《辽宁科技大学学报》
CAS
2020年第3期183-187,共5页
Journal of University of Science and Technology Liaoning
基金
国家级大学生创新创业训练计划(201910146032、201910146034、201910146037、202010146020、202010146023)
辽宁省大学生创新创业训练计划(201910146039)
国家自然科学基金重点项目(51634004)。
关键词
团簇Fe4P
成键性质
前线轨道理论
催化活性
密度泛函理论
cluster Fe4P
bonding properties
frontier orbital theory
catalytic activity
density functional theory
