铂钌团簇及电荷对甲醇活性的理论研究

doi:10.3866/PKU.WHXB201602221

Abstract

Abstract:

Density functional theory (DFT) calculations were performed to gain mechanistic insight into the methanol C―H and O―H bond activations mediated by ruthenium-doped platinum cationic clusters [Pt_nRu_m]⁺ (m + n = 3, n ≥ 1). The charge effect on the reactivity has been elucidated. Calculations show that positive charge is evenly distributed on the three Pt atoms of the [Pt₃]⁺ cluster, while in the Ru-doped clusters, positive charge is mainly distributed on the Ru atom(s). The reactivity of [Pt_nRu_m]⁺ is significantly greater than neutral [Pt_nRu_m] during the initial C―H bond cleavage, while only [Pt₃]⁺ exhibits greater reactivity than [Pt₃] in the course of O―H bond cleavage. This study may aid in deeper understanding of C―H/O―H bond activations mediated by metal clusters.

Key words: Density functional theory, Methanol, Bond activation, Charge, Reactivity

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Jun-Feng ZHAO,Xiao-Li SUN,Xu-Ri HUANG,Ji-Lai LI. A Theoretical Study on the Reactivity and Charge Effect of PtRu Clusters toward Methanol Activation[J]. Acta Phys. -Chim. Sin. 2016, 32(5), 1175-1182. doi: 10.3866/PKU.WHXB201602221

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A Theoretical Study on the Reactivity and Charge Effect of PtRu Clusters toward Methanol Activation

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