CO Self-Promoting Oxidation on Nanosized Gold Clusters: Triangular Au-3 Active Site and CO Induced O-O Scission
文献类型：期刊论文
| 作者 | Liu, Chunyan ; Tan, Yingzi ; Lin, Sisi ; Li, Hui ; Wu, Xiaojun ; Li, Lei ; Pei, Yong ; Zeng, Xiao Cheng |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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| 出版日期 | 2013 |
| 卷号 | 135期号:7页码:2583 |
| ISSN号 | 0002-7863 |
| 中文摘要 | We have systematically studied the CO oxidation on various nanosized gold clusters with sizes ranging from 0.3 to 0.8 nm on the basis of density functional theory (DFT) calculations. A hitherto unreported trimolecular Langmuir-Hinshelwood (LH) mechanism is proposed, which offers new insights into the fundamental mechanism for CO oxidation on nanosized gold clusters. Specifically, we find that the coadsorbed CO molecule at a unique triangular Au-3 active site can act as a promoter for the scission of an O-O bond, leading to the spontaneous formation (due to extremely low energy barrier) of two CO2 molecules as product. The key step to the O-O bond scission in the OCOO* intermediate is significantly accelerated due to the electrophilic attack of the coadsorbed neighboring CO molecule on the triangular Au3 site. This new mechanism is called CO self-promoting oxidation, which can be visualized in real time from the trajectory of a Born Oppenheimer molecular dynamics (BOMD) simulation. We also find that such CO self-promoting oxidation is quite universal, as long as the triangular Au3 reaction site is available. This is demonstrated in two prototype metal oxide supported gold nanostructure systems: namely, Au-n/MgO and bilayer-Au/TiO2. The coadsorbed CO can not only serve as a promoter for its own oxidation but also promote other oxidation reactions such as styrene oxidation through expediting O-O scission on gold nanostructures. |
| 语种 | 英语 |
| 公开日期 | 2014-01-17 |
| 源URL | [http://ir.iphy.ac.cn/handle/311004/57783]  |
| 专题 | 物理研究所_物理所公开发表论文_物理所公开发表论文_期刊论文 |
| 推荐引用方式 GB/T 7714 | Liu, Chunyan,Tan, Yingzi,Lin, Sisi,et al. CO Self-Promoting Oxidation on Nanosized Gold Clusters: Triangular Au-3 Active Site and CO Induced O-O Scission[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2013,135(7):2583. |
| APA | Liu, Chunyan.,Tan, Yingzi.,Lin, Sisi.,Li, Hui.,Wu, Xiaojun.,...&Zeng, Xiao Cheng.(2013).CO Self-Promoting Oxidation on Nanosized Gold Clusters: Triangular Au-3 Active Site and CO Induced O-O Scission.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,135(7),2583. |
| MLA | Liu, Chunyan,et al."CO Self-Promoting Oxidation on Nanosized Gold Clusters: Triangular Au-3 Active Site and CO Induced O-O Scission".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 135.7(2013):2583. |
入库方式： OAI收割
来源：物理研究所
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