Pt_(10)团簇催化肉桂醛选择性加氢反应机理的研究

本文以Pt_(10)团簇作为催化剂模型,采用密度泛函理论(DFT)中的B3LYP方法,在6-31+G(d)(Pt采用贗势基组Lanl2dz)基组水平上,探讨了Pt_(10)团簇催化肉桂醛选择性加氢反应的微观反应历程.研究结果表明,Pt_(10)团簇催化肉桂醛选择性加氢反应可生成3种不同的产物,分别是3-苯基丙醛(P1)、3-苯基丙烯醇(P2)和肉桂醇(P3),每种产物分别通过两条不同的反应通道而得到.Pt_(10)团簇催化有利于肉桂醛分子中C=O键活化加氢.这点与实验结果一致.

Investigation on the Mechanisms for the Selective Hydrogenation Reaction of Cinnamaldehyde Catalyzed by Pt10 Clusters

in this paper, by the means of B3LYP in DFT at 6-31+G(d) level (the LanL2DZ extra basis set was used for Pt atom) we study separately the selective hydrogenation micro reaction mechanism for Cinnamaldehyde catalyzed by Pt10 clusters. The rationality of transient state can be proved by vibration frequency analysis and IRC computation. Moreover, Atoms in molecules (AIM) theory and nature bond orbital (NBO) theory have been applied to discussing the interaction among orbits and the bonding characteristics. The results indicate that there are three kinds of products namely that 3-phenylpropyl aldehyde, 3-phenyl allyl alcohol and cinnamyl alcohol produced in the selective hydrogenation reaction catalyzed by Pt10 clusters and each pathway owns two reaction channels. Ptn clusters are more likely to catalyze the activation and hydrogenation of the C=O bond in Cinnamaldehyde molecules eventually to produce cinnamic alcohol. which is in good agreement with the experimental results.