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文章编号： 1672-6987（2022）06-0031-09； DOI： 10.16351/j.1672-6987.2022.06.005
郑新喜， 方志刚*， 秦渝， 侯欠欠， 许友
（辽宁科技大学 化学工程学院，辽宁 鞍山 114051）
摘要： 为探究团簇Fe3Ni3优化构型的热力学稳定性，并研究其催化析氢性能，在密度泛函理论中的B3LYP/Lanl2dz（level）下，利用Gaussian软件对构型进行全参数优化计算后，从各优化构型的热力学能量分析中发现：团簇Fe3Ni3共有9种优化稳定构型，包括5种三重态构型与4种单重态构型，并且三重态优化构型均相较于单重态构型具有更高的稳定性。设计团簇Fe3Ni3催化析氢具体反应机理，利用前线轨道理论在两步反应中进行分析发现，团簇Fe3Ni3所有构型均能参与水分子的催化反应，其中Fe原子是催化的主要活性位点，且构型1(1)与构型2(1)反应活性最好。
关键词： 密度泛函理论; 团簇Fe3Ni3; 前线轨道理论; 催化析氢
中图分类号： O 641.12文献标志码： A
引用格式： 郑新喜， 方志刚， 秦渝，等. 团簇Fe3Ni3稳定性及催化析氢性能［J］. 青岛科技大学学报(自然科学版), 2022, 43(6): 31-39.
ZHENG Xinxi, FANG Zhigang, QIN Yu, et al. Study on the catalytic performance of cluster Fe3Ni3 for hydrogen evolution［J］. Journal of Qingdao University of Science and Technology（Natural Science Edition), 2022, 43(6): 31-39.
Study on the Catalytic Performance of Cluster Fe3Ni3 for Hydrogen Evolution
ZHENG Xinxi, FANG Zhigang, QIN Yu, HOU Qianqian, XU You
（School of Chemical Engineering, Liaoning University of Science and Technology, Anshan 114051, China）
Abstract: In order to explore the thermodynamic stability of the optimized configuration of cluster Fe3Ni3 and study its catalytic hydrogen evolution performance, under the B3LYP / Lanl2dz (level) of density functional theory, the configuration is optimized by using Gaussian software. After the calculation, the thermodynamic energy analysis of each optimized configuration shows that: ClusterFe3Ni3 has 9 optimized stable configurations, including 5 triplet configurations and 4 singlet configurations, and the triplet optimized configurations have higher stability than the singlet configuration.The specific reaction mechanism of cluster Fe3Ni3 catalyzing hydrogen evolution was designed, and the front-line orbital theory was used to analyze the two-step reaction. It was found that all configurations of cluster Fe3Ni3 could participate in the catalytic reaction of water molecules, among which Fe atom was the main active site, and the reaction activity of configuration 1(1) and configuration 2(1) was the best.
Key words: density functional theory; cluster Fe3Ni3; frontier molecular orbit theory; catalytic hydrogen evolution
收稿日期： 2021-12-13
基金项目： 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（202010146009，202010146016)；辽宁省大学生创新创业训练计划项目（202010146059，202010146052，202010146015).
作者简介： 郑新喜（2000—），男，助理研究员.*通信联系人.
