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Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina

  • Yutong Zhao
    Yutong Zhao
    School of Engineering, Macquarie University, Sydney, New South Wales 2109, Australia
    More by Yutong Zhao
  • Lizhuo Wang
    Lizhuo Wang
    Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia
    More by Lizhuo Wang
  • Alena Kochubei
    Alena Kochubei
    School of Engineering, Macquarie University, Sydney, New South Wales 2109, Australia
  • Wenjie Yang
    Wenjie Yang
    Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia
    More by Wenjie Yang
  • Haimei Xu
    Haimei Xu
    School of Engineering, Macquarie University, Sydney, New South Wales 2109, Australia
    More by Haimei Xu
  • Yongming Luo
    Yongming Luo
    Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China
    More by Yongming Luo
  • Alfons Baiker
    Alfons Baiker
    Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zürich, Hönggerberg, HCI, Zurich CH-8093, Switzerland
  • Jun Huang
    Jun Huang
    Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia
    More by Jun Huang
  • Zichun Wang*
    Zichun Wang
    School of Engineering, Macquarie University, Sydney, New South Wales 2109, Australia
    *Email: [email protected]
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  • , and 
  • Yijiao Jiang*
    Yijiao Jiang
    School of Engineering, Macquarie University, Sydney, New South Wales 2109, Australia
    *Email: [email protected]
    More by Yijiao Jiang
Cite this: J. Phys. Chem. Lett. 2021, 12, 10, 2536–2546
Publication Date (Web):March 8, 2021
https://doi.org/10.1021/acs.jpclett.1c00139
Copyright © 2021 American Chemical Society

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    Abstract

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    Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal–support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. Pt single sites supported on AlV-enriched ASA exhibit excellent chemoselectivity in the hydrogenation of C═O groups, affording 2–3-fold higher yields compared to those of Pt nanoparticles supported on Al2O3 and SiO2.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.1c00139.

    • XRD patterns, STEM images, EELS spectra, 1H MAS NMR spectra, XPS spectra, and simulation parameters and results of 27Al and 1H MAS NMR spectra and XPS spectra (PDF)

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