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Crystal-Plane-Controlled Selectivity of Cu2O Catalysts in Propylene Oxidation with Molecular Oxygen

Authors

  • Qing Hua,

    1. Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China, Jinzhai Road 96, Hefei 230026 (China)
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    • These authors contributed equally.

  • Tian Cao,

    1. Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China, Jinzhai Road 96, Hefei 230026 (China)
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    • These authors contributed equally.

  • Dr. Xiang-Kui Gu,

    1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023 (China)
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    • These authors contributed equally.

  • Prof. Dr. Jiqing Lu,

    1. Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004 (China)
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    • These authors contributed equally.

  • Dr. Zhiquan Jiang,

    1. Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China, Jinzhai Road 96, Hefei 230026 (China)
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  • Xiaorong Pan,

    1. Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004 (China)
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  • Liangfeng Luo,

    1. Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China, Jinzhai Road 96, Hefei 230026 (China)
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  • Prof. Dr. Wei-Xue Li,

    1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023 (China)
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  • Prof. Dr. Weixin Huang

    Corresponding author
    1. Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China, Jinzhai Road 96, Hefei 230026 (China)
    • Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China, Jinzhai Road 96, Hefei 230026 (China)===

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  • This research was financially supported by the National Natural Science Foundation of China (21173204, 11079033, 21225315), the National Basic Research Program of China (2013CB933104, 2010CB923301), and the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA09030103).

Abstract

The selective oxidation of propylene with O2 to propylene oxide and acrolein is of great interest and importance. We report the crystal-plane-controlled selectivity of uniform capping-ligand-free Cu2O octahedra, cubes, and rhombic dodecahedra in catalyzing propylene oxidation with O2: Cu2O octahedra exposing {111} crystal planes are most selective for acrolein; Cu2O cubes exposing {100} crystal planes are most selective for CO2; Cu2O rhombic dodecahedra exposing {110} crystal planes are most selective for propylene oxide. One-coordinated Cu on Cu2O(111), three-coordinated O on Cu2O(110), and two-coordinated O on Cu2O(100) were identified as the catalytically active sites for the production of acrolein, propylene oxide, and CO2, respectively. These results reveal that crystal-plane engineering of oxide catalysts could be a useful strategy for developing selective catalysts and for gaining fundamental understanding of complex heterogeneous catalytic reactions at the molecular level.

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