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Multiscale Visualization and Quantification of the Effect of Binders on the Acidity of Shaped Zeolites

  • Koen Kennes
    Koen Kennes
    Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions, Faculty of Bioscience Engineering, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
    More by Koen Kennes
  • Alexey Kubarev
    Alexey Kubarev
    Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions, Faculty of Bioscience Engineering, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
  • Coralie Demaret
    Coralie Demaret
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
  • Laureline Treps
    Laureline Treps
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
  • Olivier Delpoux
    Olivier Delpoux
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
  • Mickael Rivallan
    Mickael Rivallan
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
  • Emmanuelle Guillon
    Emmanuelle Guillon
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
  • Alain Méthivier
    Alain Méthivier
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
  • Theodorus de Bruin
    Theodorus de Bruin
    IFP Energies nouvelles, 1 et 4 Avenue de Bois-Préau, BP3, 92852 Rueil-Malmaison, France
  • Axel Gomez
    Axel Gomez
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
    Département de Chimie, École Normale Supérieure, PSL University, 75005 Paris, France
    More by Axel Gomez
  • Bogdan Harbuzaru
    Bogdan Harbuzaru
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
  • Maarten B.J. Roeffaers*
    Maarten B.J. Roeffaers
    Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions, Faculty of Bioscience Engineering, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
    *Email: [email protected]
  • , and 
  • Céline Chizallet*
    Céline Chizallet
    IFP Energies nouvelles, Rond-Point de L’Echangeur de Solaize, BP 3 69360 Solaize, France
    *Email: [email protected]
Cite this: ACS Catal. 2022, 12, 11, 6794–6808
Publication Date (Web):May 24, 2022
https://doi.org/10.1021/acscatal.2c02152
Copyright © 2022 American Chemical Society

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    Abstract

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    Shaping is a crucial step in the preparation of catalysts at the industrial scale, but a rationalized understanding of how binders impact the catalyst’s performance is still far from apparent. In this work, the effect of shaping with common binders (boehmite, γ-Al2O3, and silica) on the acidity and catalytic properties of an acid zeolite catalyst, H-ZSM-5, is probed. The zeolite–binder samples (1:1 ratio) are shaped following commonly employed procedures and analyzed using both conventional characterizations of the acidity and porosity as well as using advanced fluorescence microspectroscopic characterization. In the latter approach, the fluorescence intensity stemming from the Brønsted acid-catalyzed furfuryl alcohol oligomerization is used to determine in detail the effect of shaping on acid zeolite’s catalytic activity. Through density functional theory calculations, the observed changes in catalytic performance are assigned to atomic-scale processes such as the interaction of acid sites with binder-related molecular species and the migration of ions. The most detrimental effects related to shaping are migration of cations, here Na+, from the binder to the zeolite, which is an important mechanism for silica binders, as well as pore blockage by alumina and silica species. Strong acid sites are also likely to be converted into weak ones upon interaction with binders. A counterbalancing effect is the genesis of some additional bridging OH groups upon filling of local defects with alumina species from alumina binders. With such knowledge in hand, it becomes possible to balance these effects to get the desired properties.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.2c02152.

    • Physisorption isotherms; IR spectra; xylene isomerization; and DFT calculations (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Yuanyuan Gao, Yijun Zhang, Laure Michelin, Jacques Lalevée, Angélique Simon-Masseron. Binder effects in photopolymerized acrylate/zeolite composites for 3D printing/ion-exchange applications. Materials Chemistry and Physics 2023, 293 , 126853. https://doi.org/10.1016/j.matchemphys.2022.126853

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