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; Zheng, XS; Zhu, JF; Zhang, WH; Ma, C; Si, R; Zeng, J; 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.; Zeng, J (reprint author), Univ Sci & Technol China, Dept Chem Phys, Natl Synchrotron Radiat Lab, Hefei 230026, Peoples R China.
2016
发表期刊NATURE COMMUNICATIONS
ISSN2041-1723
卷号7页码:-
文章类型期刊论文
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.
DOI10.1038/ncomms14036
收录类别SCI
语种英语
WOS记录号WOS:000390286100001
引用统计
文献类型期刊论文
条目标识符http://ir.sinap.ac.cn/handle/331007/26434
专题中科院上海应用物理研究所2011-2018年
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.; Zeng, J (reprint author), Univ Sci & Technol China, Dept Chem Phys, Natl Synchrotron Radiat Lab, Hefei 230026, Peoples R China.
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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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