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Differentiating Surface Ce Species among CeO2 Facets by Solid-State NMR for Catalytic Correlation

  • Zicong Tan
    Zicong Tan
    Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong 999077, P. R. China
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  • Guangchao Li
    Guangchao Li
    State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, P. R. China
    University of Chinese Academy of Sciences, Beijing 100049, P. R. China
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  • Hung-Lung Chou*
    Hung-Lung Chou
    Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, Taipei 10617, Taiwan
    *E-mail: [email protected] (H.-L.C.).
  • Yiyang Li
    Yiyang Li
    The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford, Oxford OX1 3QR, U.K.
    More by Yiyang Li
  • Xianfeng Yi
    Xianfeng Yi
    State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, P. R. China
    More by Xianfeng Yi
  • Abdul Hanif Mahadi
    Abdul Hanif Mahadi
    Centre for Advanced Material and Energy Sciences, Universiti Brunei Darussalam, Gadong 1410, Negara Brunei Darussalam
  • Anmin Zheng*
    Anmin Zheng
    State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, P. R. China
    School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, Henan 450052, P. R. China
    *E-mail: [email protected] (A.Z.).
    More by Anmin Zheng
  • Shik Chi Edman Tsang
    Shik Chi Edman Tsang
    The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford, Oxford OX1 3QR, U.K.
  • , and 
  • Yung-Kang Peng*
    Yung-Kang Peng
    Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong 999077, P. R. China
    *E-mail: [email protected] (Y.-K.P.).
Cite this: ACS Catal. 2020, 10, 7, 4003–4011
Publication Date (Web):March 4, 2020
https://doi.org/10.1021/acscatal.0c00014
Copyright © 2020 American Chemical Society
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Abstract

Altering the exposed facet of CeO2 nanocrystallites and hence the control of surface chemistry on the nano level have been shown to significantly change their performances in various catalytic reactions. The chemical state of surface Ce, which is associated with Lewis acidity and hence the adsorption/activation energy of reactants on the surface, is expected to vary with their hosted facets. Unfortunately, traditional surface tools fail to differentiate/quantify them among hosted facets and thus have led to different interpretations among researchers in the past decades. Herein, probe-assisted nuclear magnetic resonance is employed for the surface investigation of different CeO2 facets. They not only allow differentiation of the surface Ce atoms between hosted facets at high resolution but can also provide their corresponding concentrations. The as-established facet fingerprint of CeO2 can thus report on the facet distribution/concentration of a given CeO2 sample. Dephosphorylation and H2O2 reduction were tested as probe reactions to demonstrate the importance of obtaining comprehensive surface Ce information for the active site identification and the rational design of CeO2-based catalysts. Around 1000 and 4500% increase in activity of those reactions can be easily achieved on pristine CeO2 without further surface engineering when its terminal facet is wisely chosen. Our results thus imply that the basic surface knowledge of even a simple catalyst can be more important than the continuous development of their fancy derivatives without clear guidance.

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  • Experimental details for quantitative 31P MAS NMR and XRD, XPS, Raman, DFT calculation, and additional catalytic study on CeO2 morphologies (PDF)

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