[1]郑新喜,方志刚*,侯欠欠,等.团簇Fe3Ni3的极化率与催化性质[J].江西师范大学学报(自然科学版),2021,(05):473-479.[doi:10.16357/j.cnki.issn1000-5862.2021.05.05]
　ZHENG Xinxi,FANG Zhigang*,HOU Qianqian,et al.The Polarizability and Catalytic Properties of Cluster Fe3Ni3[J].Journal of Jiangxi Normal University:Natural Science Edition,2021,(05):473-479.[doi:10.16357/j.cnki.issn1000-5862.2021.05.05]
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团簇Fe3Ni3的极化率与催化性质()
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《江西师范大学学报》（自然科学版）[ISSN:1006-6977/CN:61-1281/TN]

卷:
期数:
2021年05期
页码:
473-479
栏目:
出版日期:
2021-10-10

文章信息/Info

Title:
The Polarizability and Catalytic Properties of Cluster Fe3Ni3
文章编号:
1000-5862(2021)05-0473-07
作者:
郑新喜; 方志刚*; 侯欠欠; 吕孟娜; 井润田
辽宁科技大学化学工程学院,辽宁 鞍山 114051
Author(s):
ZHENG Xinxi; FANG Zhigang*; HOU Qianqian; LYU Mengna; JING Runtian
School of Chemical Engineering,University of Science and Technology Liaoning,Anshan Liaoning 114051,China
关键词:
密度泛函理论;  极化率;  前线轨道理论;  催化性质;  费米能级
Keywords:
density functional theory;  polarizability;  frontier molecular orbital theory;  catalytic properties;  fermi level
分类号:
O 641.12
DOI:
10.16357/j.cnki.issn1000-5862.2021.05.05
文献标志码:
A
摘要:
为探究团簇Fe3Ni3优化构型的稳定性及其受外场影响的形变情况,并研究其催化性质,使用密度泛函理论中的B3LYP/Lanl2dz(Level)对设计出的初始构型进行全参数优化计算,将含虚频和能量较高的相同构型排除后,最终得到9种稳定的优化构型.从各优化构型的极化率、前线轨道及福井函数分析发现:构型4(3)的极化率最大,原子间的相互作用力最小,构型易发生形变,且构型4(3)的能隙差最小,电子从HOMO轨道向LUMO轨道转移的难度最小,在催化反应过程中反应活性最好; 单重态构型比三重态构型原子间相互作用力更强,结构更致密,不易发生形变; 在三重态构型中Fe原子是前线轨道的主要贡献者,是催化反应过程中的潜在活性位点,具有较强的得电子能力.而单重态构型与之相反,Ni原子是前线轨道的主要贡献者,在催化过程中提供电子的能力较强.
Abstract:
In order to explore the stability of the optimized configuration of clusters Fe3Ni3 and the deformations affected by external fields,and to study its catalytic properties,B3LYP/Lanl2dz(Level)in density functional theory is used to perform full parameter optimization calculations on the designed initial configurations.After excluding configurations with false frequency and the same higher energy,9 stable optimized configurations are finally obtained.From the analysis of the polarizability,frontier molecular orbital theory and Fukui function of each optimized configuration,it is found that the polarizability of configuration 4(3) is the largest,the interaction force between atoms of it is the smallest,thus this configuration is prone to deformation,and the energy gap difference is the smallest,transfer of electrons from the HOMO orbit to the LUMO orbit is the least difficult,it has the best reactivity in the process of catalytic reaction.Compared with the triplet configurations,the interaction between atoms is stronger,the structure is denser,and it is not easy to deform.In the triplet configurations,the Fe atom is the main contributor to the frontier orbital,so it is a potential active siteof clusters Fe3Ni3 in the catalytic reaction process,and it has a strong ability to obtain electrons,while the singlet configurations are the Ni atom.The main contributor to the frontline orbit has a strong ability to provide electrons in the catalytic process.

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备注/Memo

备注/Memo:
收稿日期:2021-05-14
基金项目:国家自然科学基金(51634004),国家级大学生创新创业训练计划(202010146009,202010146016)和辽宁省大学生创新创业训练计划(202110146056,202110146049,202110146040)资助项目.
通信作者:方志刚(1964—),男,辽宁鞍山人,教授,博士,博士生导师,主要从事量子化学、物理化学及表面催化研究.E-mail:lnfzg@163.com
更新日期/Last Update: 2021-10-10