团簇Mo2S4的催化析氢活性计算分析

利用Gaussian 09程序对团簇Mo₂S₄进行全参数的优化计算，根据前线轨道理论对计算所得的10种稳定构型进行催化析氢反应活性的研究，由前线轨道图及团簇Mo₂S₄与水分子的前线轨道能级差探究团簇Mo₂S₄在催化水解析氢中的反应活性，进而确定团簇Mo₂S₄催化析氢活性最好的理论模型。结果表明，团簇Mo₂S₄单重态构型的稳定性优于三重态构型，三重态构型催化水解析氢的能力相较于单重态构型更占优势；构型5^（3）在吸附氢原子与解吸氢原子的反应中都有较好的反应活性，构型4^（1）的反应活性最弱。

Calculation and analysis of the catalytic hydrogen evolution activity of the Mo2S4 cluster

The Gaussian 09 program has been used to optimize the full parameters of the Mo₂S₄ cluster. According to frontier molecular orbital theory, the catalytic hydrogen evolution reaction activities of the 10 stable configurations were studied. From the frontier orbital diagrams and the frontier orbital energy differences between the Mo₂S₄ cluster and water molecules, the activity of the Mo₂S₄ cluster in catalytic hydrogen evolution from water was explored, and a theoretical model of the best catalytic activity for hydrogen evolution with an Mo₂S₄ cluster was determined. The results show that the stability of the Mo₂S₄ singlet configuration is better than that of triplet configuration. The activity of the triplet configuration in the catalytic hydrogen evolution reaction is higher than that of the singlet configuration. The triplet configuration 5⁽³⁾ has good activity in terms of adsorbing and desorbing hydrogen atoms, whilst the singlet configuration 4⁽¹⁾ has the lowest activity.