基于密度泛函理论的团簇Co2Mo2P3催化性质研究

doi:10.16088/j.issn.1001-6600.2024032001

摘要/Abstract

摘要： 基于拓扑学原理和密度泛函理论,本文探究团簇Co₂Mo₂P₃的催化反应作用机理及其活性产生的原因,使用Gaussian09程序,在B3LYP/Lanl2dz水平下,对团簇的初始构型进行全参数优化和运算分析。对Co₂Mo₂P₃中各个原子对其HOMO和LUMO轨道的贡献进行研究,得到Co对其前线轨道的贡献率为53.511%、59.013%,Co原子在该团簇中是潜在的活性位点。通过观察态密度图和HOMO-LUMO图,发现Co原子是引起费米能量级两边峰值的主要因素。进一步的能隙差和库普曼斯定理分析显示,构型1⁽⁴⁾和3⁽⁴⁾具有较强的得失电子能力,并且拥有比其他构型更强的催化活性,这些结果为深入理解团簇Co₂Mo₂P₃的催化性能提供了有力支持。本研究的发现为团簇Co₂Mo₂P₃在催化反应中的应用机制和活性产生的原因提供了重要理论依据,为进一步优化催化性能,设计高效催化剂提供了有益参考。

关键词: 团簇Co₂Mo₂P₃, 密度泛函理论, 前线轨道, 催化性质, 态密度, 能隙差, 库普曼斯定理

Abstract: Based on topological principles and density functional theory,the catalytic reaction mechanism and the reasons behind the activity of the Co₂Mo₂P₃ cluster were investigated. Using the Gaussian09 program at the B3LYP/Lanl2dz level,full parameter optimization and computational analysis of the cluster's initial configuration were performed. Through an analysis of the contributions of each atom in the Co₂Mo₂P₃ cluster to the HOMO and LUMO orbitals,we found that the Co atoms contribute 53.511% and 59.013% to the frontier orbitals,indicating their potential as active sites in the cluster. Additionally,observations of the density of states and HOMO-LUMO plots revealed that the Co atoms played a significant role in generating the peaks in the Fermi energy levels. Further analysis of the energy gap and Koopmans' theorem showed that configurations 1⁽⁴⁾ and 3⁽⁴⁾ had strong electron-gaining and electron-donating capabilities,respectively,and possess higher catalytic activity compared with other configurations. These results provide robust support for a deeper understanding of the catalytic performance of the Co₂Mo₂P₃ cluster. The findings of this study offer essential theoretical insights into the catalytic reaction mechanism and activity generation of the Co₂Mo₂P₃ cluster,providing valuable references for further optimizing catalytic performance and designing efficient catalysts.

Key words: Co₂Mo₂P₃ cluster, density functional theory, front-line tracks, catalytic properties, state density, energy gap, Koopmans' theorem

中图分类号: O641.12

吴庭慧, 方志刚, 刘立娥, 宋静丽, 宋嘉. 基于密度泛函理论的团簇Co₂Mo₂P₃催化性质研究[J]. 广西师范大学学报（自然科学版）, 2024, 42(5): 141-149.

WU Tinghui, FANG Zhigang, LIU Li'e, SONG Jingli, SONG Jia. Catalytic Properties of Co₂Mo₂P₃ Cluster Analyzed by Density Functional Theory[J]. Journal of Guangxi Normal University(Natural Science Edition), 2024, 42(5): 141-149.

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基于密度泛函理论的团簇Co₂Mo₂P₃催化性质研究

Catalytic Properties of Co₂Mo₂P₃ Cluster Analyzed by Density Functional Theory

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