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

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

1.
Institute of Theoretical Chemistry, Jilin University, Changchun 130023, P. R. China

Corresponding author: LI Ji-Lai,
Received Date: 6 October 2015
Available Online: 22 February 2016
Fund Project: 国家重点基础研究发展规划项目(973)(2012CB932800) (973)(2012CB932800)国家自然科学基金(21103064,21473070)资助 (21103064,21473070)

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.
- Density functional theory,
- Methanol,
- Bond activation,
- Charge,
- Reactivity
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