Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst

Liangbing Wang, Wenbo Zhang, Shenpeng Wang, Zehua Gao, Zhiheng Luo, Xu Wang, Rui Zeng, Aowen Li, Hongliang Li, Menglin Wang, Xusheng Zheng, Junfa Zhu, Wenhua Zhang (), Chao Ma (), Rui Si and Jie Zeng ()
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Liangbing Wang: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wenbo Zhang: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Shenpeng Wang: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Zehua Gao: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Zhiheng Luo: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Xu Wang: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Rui Zeng: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Aowen Li: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Hongliang Li: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Menglin Wang: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Xusheng Zheng: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Junfa Zhu: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wenhua Zhang: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Chao Ma: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China
Rui Si: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Jie Zeng: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Hefei Science Center & National Synchrotron Radiation Laboratory, University of Science and Technology of China

Nature Communications, 2016, vol. 7, issue 1, 1-8

Abstract: Abstract 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.

Date: 2016
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DOI: 10.1038/ncomms14036

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