Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst | |
Wang, LB; Zhang, WB; Wang, SP; Gao, ZH; Luo, ZH; Wang, X; Zeng, R; Li, AW; Li, HL; Wang, ML | |
刊名 | NATURE COMMUNICATIONS |
2016 | |
卷号 | 7页码:- |
ISSN号 | 2041-1723 |
通讯作者 | Zhang, WH ; Ma, C ; Zeng, J (reprint author), Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Key Lab Strongly Coupled Quantum Matter Phys, Chinese Acad Sci,Hefei Sci Ctr, Hefei 230026, Peoples R China. ; Zhang, WH ; Ma, C ; Zeng, J (reprint author), Univ Sci & Technol China, Dept Chem Phys, Natl Synchrotron Radiat Lab, Hefei 230026, Peoples R China. |
英文摘要 | Rh-based heterogeneous catalysts generally have limited selectivity relative to their homogeneous counterparts in hydroformylation reactions despite of the convenience of catalyst separation in heterogeneous catalysis. Here, we develop CoO-supported Rh single-atom catalysts (Rh/CoO) with remarkable activity and selectivity towards propene hydroformylation. By increasing Rh mass loading, isolated Rh atoms switch to aggregated clusters of different atomicity. During the hydroformylation, Rh/CoO achieves the optimal selectivity of 94.4% for butyraldehyde and the highest turnover frequency number of 2,065 h(-1) among the obtained atomic-scale Rh-based catalysts. Mechanistic studies reveal that a structural reconstruction of Rh single atoms in Rh/CoO occurs during the catalytic process, facilitating the adsorption and activation of reactants. In kinetic view, linear products are determined as the dominating products by analysing reaction paths deriving from the two most stable co-adsorbed configurations. As a bridge of homogeneous and heterogeneous catalysis, single-atom catalysts can be potentially applied in other industrial reactions. |
收录类别 | SCI |
语种 | 英语 |
WOS记录号 | WOS:000390286100001 |
内容类型 | 期刊论文 |
源URL | [http://ir.sinap.ac.cn/handle/331007/26434] |
专题 | 上海应用物理研究所_中科院上海应用物理研究所2011-2017年 |
推荐引用方式 GB/T 7714 | Wang, LB,Zhang, WB,Wang, SP,et al. Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst[J]. NATURE COMMUNICATIONS,2016,7:-. |
APA | Wang, LB.,Zhang, WB.,Wang, SP.,Gao, ZH.,Luo, ZH.,...&Zeng, J.(2016).Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst.NATURE COMMUNICATIONS,7,-. |
MLA | Wang, LB,et al."Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst".NATURE COMMUNICATIONS 7(2016):-. |
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