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Pt–ZnOx Interfacial Effect on the Performance of Propane Dehydrogenation and Mechanism Study
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    Pt–ZnOx Interfacial Effect on the Performance of Propane Dehydrogenation and Mechanism Study
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    • Daoru Liu
      Daoru Liu
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
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    • Feifei Jiang
      Feifei Jiang
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
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    • Qinghua Zhang
      Qinghua Zhang
      Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
    • Wei-Hsiang Huang
      Wei-Hsiang Huang
      National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan
      Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology (NTUST), Taipei 10607, Taiwan
    • Yanping Zheng
      Yanping Zheng
      State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
    • Mingshu Chen
      Mingshu Chen
      State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
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    • Liming Wu
      Liming Wu
      State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
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    • Ruixuan Qin
      Ruixuan Qin
      State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
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    • Mingzhi Wang
      Mingzhi Wang
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
      More by Mingzhi Wang
    • Shiyi Zhang
      Shiyi Zhang
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
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    • Limin Chen
      Limin Chen
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
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    • Keyou Yan
      Keyou Yan
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
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    • Linan Zhou
      Linan Zhou
      Spin-X Institute, School of Chemistry and Chemical Engineering, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510641, China
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    • Yun Zhao*
      Yun Zhao
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
      *Email: [email protected]
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    • Lin Gu*
      Lin Gu
      Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
      School of Materials Science and Engineering, Tsinghua University, Beijing 100083, China
      *Email: [email protected]
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    • Guangxu Chen*
      Guangxu Chen
      School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510006, China
      *Email: [email protected]
      More by Guangxu Chen
    Other Access OptionsSupporting Information (1)

    ACS Nano

    Cite this: ACS Nano 2024, 18, 51, 34671–34682
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c10030
    Published December 11, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    Bimetallic Pt-based catalysts, for example, PtZn and PtSn catalysts, have gained significant attention for addressing the poor stability and low selectivity of pristine Pt catalysts over propane dehydrogenation (PDH). However, the structures of the active sites and the corresponding catalytic mechanism of PDH are still elusive. Here, we demonstrate a spatially confined Pt–ZnmOx@RUB-15 catalyst (where “m” is the mole ratio of Zn/Pt and RUB-15 is a layered silica), which exhibited high catalytic activity, ultrahigh selectivity (>99%), and resistance to coking at 550 °C for PDH. Significantly different from the preliminary studies over the PtZn catalysts, through the assistance of quasi-in situ X-ray photoelectron spectroscopy (XPS), in situ Fourier transform infrared spectroscopy (CO-FTIR), in situ X-ray absorption spectroscopy (XAS), and CO titration, we discovered that the active sites for PDH were the Pt–ZnOx interfaces, characterized by a structure of Ptδ+–Zn2+–O–Si. Density functional theory (DFT) calculations showed that Pt atoms positioned at Pt–ZnOx interfaces with coordinatively unsaturated ZnOx sites facilitate the C–H bond breaking of propane while concurrently suppressing deep dehydrogenation processes. This study suggests that engineering the interfaces of Pt–metal oxides under spatially confined conditions holds promise for developing highly efficient Pt-based catalysts for light alkane dehydrogenation.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.4c10030.

    • Additional SEM, TEM, STEM, EDS mapping, AC-HAADF-STEM images; XRD patterns; XPS spectra; XAS spectra; catalytic measurement details; computational details; characterization details; and additional experimental and computational results (PDF)

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    ACS Nano

    Cite this: ACS Nano 2024, 18, 51, 34671–34682
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c10030
    Published December 11, 2024
    Copyright © 2024 American Chemical Society

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