基于密度泛函理论的团簇Co_(2)Mo_(2)P_(3)催化性质研究  

Catalytic Properties of Co_(2)Mo_(2)P_(3)Cluster Analyzed by Density Functional Theory

作　　者：吴庭慧 方志刚[1] 刘立娥 宋静丽 宋嘉 WU Tinghui;FANG Zhigang;LIU Li’e;SONG Jingli;SONG Jia(School of Chemical Engineering,Liaoning University of Science and Technology,Anshan Liaoning 114051,China)

机构地区：[1]辽宁科技大学化学工程学院,辽宁鞍山114051

出　　处：《广西师范大学学报（自然科学版）》2024年第5期141-149,共9页Journal of Guangxi Normal University:Natural Science Edition

基　　金：国家自然科学基金重点项目(51634004);国家级大学生创新创业训练计划项目(202310146026,202310146027,202310146025)。

摘　　要：基于拓扑学原理和密度泛函理论,本文探究团簇Co_(2)Mo_(2)P_(3)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Co_(2)Mo_(2)P_(3)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Co_(2)Mo_(2)P_(3)的催化性能提供了有力支持。本研究的发现为团簇Co_(2)Mo_(2)P_(3)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。Based on topological principles and density functional theory,the catalytic reaction mechanism and the reasons behind the activity of the Co_(2)Mo_(2)P_(3)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 Co_(2)Mo_(2)P_(3)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 Co_(2)Mo_(2)P_(3)cluster.The findings of this study offer essential theoretical insights into the catalytic reaction mechanism and activity generation of the Co_(2)Mo_(2)P_(3)cluster,providing valuable references for further optimizing catalytic performance and designing efficient catalysts.

关 键 词：团簇Co_(2)Mo_(2)P_(3) 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 

分 类 号：O641.12[理学—物理化学]