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The Porosity, Acidity, and Reactivity of Dealuminated Zeolite ZSM-5 at the Single Particle Level: The Influence of the Zeolite Architecture

Authors

  • Luis R. Aramburo,

    1. Inorganic Chemistry and Catalysis, Debye Institute for NanoMaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht (The Netherlands), Fax: (+31) 30-251-1027
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    • These authors equally contributed to this work.

  • Dr. Lukasz Karwacki,

    1. Inorganic Chemistry and Catalysis, Debye Institute for NanoMaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht (The Netherlands), Fax: (+31) 30-251-1027
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    • These authors equally contributed to this work.

  • Dr. Pablo Cubillas,

    1. Centre for Nanoporous Materials, School of Chemistry, The University of Manchester, Oxford Road, Manchester M13 9 LP (UK)
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  • Shunsuke Asahina,

    1. European Application Group, JEOL (Europe) SAS Espace Claude Monet allbe de Givemy 78290 Croissy-Sur-Seine (France)
    2. Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577 (Japan)
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  • D. A. Matthijs de Winter,

    1. Biomolecular Imaging, Faculty of Science, Utrecht University, 3584 CH Utrecht (The Netherlands)
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  • Prof. Martyn R. Drury,

    1. Department of Earth Sciences, Faculty of Geosciences, Utrecht University, 3508 TA Utrecht (The Netherlands)
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  • Inge L. C. Buurmans,

    1. Inorganic Chemistry and Catalysis, Debye Institute for NanoMaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht (The Netherlands), Fax: (+31) 30-251-1027
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  • Dr. Eli Stavitski,

    1. Inorganic Chemistry and Catalysis, Debye Institute for NanoMaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht (The Netherlands), Fax: (+31) 30-251-1027
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  • Davide Mores,

    1. Inorganic Chemistry and Catalysis, Debye Institute for NanoMaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht (The Netherlands), Fax: (+31) 30-251-1027
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  • Prof. Marco Daturi,

    1. Laboratoire Catalyse et Spectrochimie, 6 Boulevard Marechal Juin, 14050 Caen (France)
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  • Philippe Bazin,

    1. Laboratoire Catalyse et Spectrochimie, 6 Boulevard Marechal Juin, 14050 Caen (France)
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  • Dr. Paul Dumas,

    1. Synchrotron SOLEIL, L'Orme des Merisiers Saint-Aubin - BP4891192, Gif-sur-Yvette Cedex (France)
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  • Prof. Fréderic Thibault-Starzyk,

    1. Laboratoire Catalyse et Spectrochimie, 6 Boulevard Marechal Juin, 14050 Caen (France)
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  • Dr. Jan A. Post,

    1. Biomolecular Imaging, Faculty of Science, Utrecht University, 3584 CH Utrecht (The Netherlands)
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  • Prof. Michael W. Anderson,

    1. Centre for Nanoporous Materials, School of Chemistry, The University of Manchester, Oxford Road, Manchester M13 9 LP (UK)
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  • Prof. Osamu Terasaki,

    1. Graduate School of EEWS (WCU), KAIST, Daejeon 305-701 (Korea)
    2. Department of Materials & Environmental Chemistry, Stockholm University, 10691 Stockholm (Sweden)
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  • Prof. Bert M. Weckhuysen

    Corresponding author
    1. Inorganic Chemistry and Catalysis, Debye Institute for NanoMaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht (The Netherlands), Fax: (+31) 30-251-1027
    • Inorganic Chemistry and Catalysis, Debye Institute for NanoMaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht (The Netherlands), Fax: (+31) 30-251-1027
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Abstract

A combination of atomic force microscopy (AFM), high-resolution scanning electron microscopy (HR-SEM), focused-ion-beam scanning electron microscopy (FIB-SEM), X-ray photoelectron spectroscopy (XPS), confocal fluorescence microscopy (CFM), and UV/Vis and synchrotron-based IR microspectroscopy was used to investigate the dealumination processes of zeolite ZSM-5 at the individual crystal level. It was shown that steaming has a significant impact on the porosity, acidity, and reactivity of the zeolite materials. The catalytic performance, tested by the styrene oligomerization and methanol-to-olefin reactions, led to the conclusion that mild steaming conditions resulted in greatly enhanced acidity and reactivity of dealuminated zeolite ZSM-5. Interestingly, only residual surface mesoporosity was generated in the mildly steamed ZSM-5 zeolite, leading to rapid crystal coloration and coking upon catalytic testing and indicating an enhanced deactivation of the zeolites. In contrast, harsh steaming conditions generated 5–50 nm mesopores, extensively improving the accessibility of the zeolites. However, severe dealumination decreased the strength of the Brønsted acid sites, causing a depletion of the overall acidity, which resulted in a major drop in catalytic activity.

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