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Correlating Acid Site Distribution and Catalytic Activity in Dealuminated Mordenite at the Single-Particle Level

  • Guillaume Fleury
    Guillaume Fleury
    Department of Microbial and Molecular Systems, Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions (cMACS), KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
  •  and 
  • Maarten B. J. Roeffaers*
    Maarten B. J. Roeffaers
    Department of Microbial and Molecular Systems, Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions (cMACS), KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium
    *Email: [email protected]
Cite this: ACS Catal. 2020, 10, 24, 14801–14809
Publication Date (Web):December 3, 2020
https://doi.org/10.1021/acscatal.0c04144
Copyright © 2020 American Chemical Society

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    Abstract

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    Researchers widely use bulk scale measurements to rationalize catalyst performances and construct structure–activity relationships. Such ensemble-averaged information neglects the complexity of the catalytic process, where spatial variations in molecular transport and catalytic site availability strongly influence the overall performance. However, understanding the interplay between the molecular processes and the local catalyst properties at the scale of individual particles requires the correlation of information obtained from different microscopy techniques. In this contribution, we directly reveal the nontrivial nanoscale correlation between the acid site distribution and the local catalytic performance of dealuminated mordenite zeolite particles by sequentially applying advanced Raman microspectroscopy, scanning electron microscopy, and fluorescence microscopy. In addition to the intra- and interparticle heterogeneities, the nonstraightforward correlation between acidity and activity at the pixel-to-pixel level highlights the complex impact of postsynthetic treatments on zeolites.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.0c04144.

    • Experimental details, the XRD pattern of Meso-MOR, the N2 physisorption isotherm of Meso-MOR, SRS imaging of pyridinium chemisorbed in a Meso-MOR crystal at different focal planes spaced by 1 μm, SRS and CFM images after the calcination following SEM characterization and preceding the addition of FFA, the distribution of the occurrence of points at different acid site densities, and the associated fit (PDF)

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    Cited By

    This article is cited by 13 publications.

    1. José Adán Moreno-Torres, Aurore Lecharlier, Fabricio Espejel-Ayala, Johan Hofkens, Eduard Fron, Maarten B. J. Roeffaers, Eduardo Coutino-Gonzalez, Rafael Ramírez-Bon. White-Light Emissive Silver-Exchanged Nanoporous NaP1 Zeolites. ACS Applied Nano Materials 2024, Article ASAP.
    2. Lihi Rikanati, Hadar Shema, Tzipora Ben-Tzvi, Elad Gross. Nanoimaging of Facet-Dependent Adsorption, Diffusion, and Reactivity of Surface Ligands on Au Nanocrystals. Nano Letters 2023, 23 (12) , 5437-5444. https://doi.org/10.1021/acs.nanolett.3c00250
    3. Shahar Dery, Barak Friedman, Hadar Shema, Elad Gross. Mechanistic Insights Gained by High Spatial Resolution Reactivity Mapping of Homogeneous and Heterogeneous (Electro)Catalysts. Chemical Reviews 2023, 123 (9) , 6003-6038. https://doi.org/10.1021/acs.chemrev.2c00867
    4. Weiqing Yang, Zhihong Wei, Yan Nie, Yuxi Tian. Optical Detection and Imaging of Nonfluorescent Matter at the Single-Molecule/Particle Level. The Journal of Physical Chemistry Letters 2022, 13 (41) , 9618-9631. https://doi.org/10.1021/acs.jpclett.2c02228
    5. Guillaume Fleury, Monica J. Mendoza-Castro, Noemi Linares, Maarten B. J. Roeffaers, Javier García-Martínez. Micelle Formation inside Zeolites: A Critical Step in Zeolite Surfactant-Templating Observed by Raman Microspectroscopy. ACS Materials Letters 2022, 4 (1) , 49-54. https://doi.org/10.1021/acsmaterialslett.1c00514
    6. Camilo A. Mesa, Michael Sachs, Ernest Pastor, Nicolas Gauriot, Alice J. Merryweather, Miguel A. Gomez-Gonzalez, Konstantin Ignatyev, Sixto Giménez, Akshay Rao, James R. Durrant, Raj Pandya. Correlating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging. Nature Communications 2024, 15 (1) https://doi.org/10.1038/s41467-024-47870-9
    7. Shweta Sharma, Florian Maurer, Patrick Lott, Thomas L. Sheppard. Unlocking the Mysteries of Technical Catalyst Deactivation: A View from Space. ChemCatChem 2024, 60 https://doi.org/10.1002/cctc.202301655
    8. Rafael Mayorga González, J. J. Erik Maris, Marita Wagner, Yadolah Ganjkhanlou, Johan G. Bomer, Maximilian J. Werny, Freddy T. Rabouw, Bert M. Weckhuysen, Mathieu Odijk, Florian Meirer. Fluorescent‐Probe Characterization for Pore‐Space Mapping with Single‐Particle Tracking. Angewandte Chemie International Edition 2024, 63 (4) https://doi.org/10.1002/anie.202314528
    9. Rafael Mayorga González, J. J. Erik Maris, Marita Wagner, Yadolah Ganjkhanlou, Johan G. Bomer, Maximilian J. Werny, Freddy T. Rabouw, Bert M. Weckhuysen, Mathieu Odijk, Florian Meirer. Fluorescent‐Probe Characterization for Pore‐Space Mapping with Single‐Particle Tracking. Angewandte Chemie 2024, 136 (4) https://doi.org/10.1002/ange.202314528
    10. Si Liu, Luca D'Amario, Shan Jiang, Holger Dau. Selected applications of operando Raman spectroscopy in electrocatalysis research. Current Opinion in Electrochemistry 2022, 35 , 101042. https://doi.org/10.1016/j.coelec.2022.101042
    11. Sophie H van Vreeswijk, Bert M Weckhuysen. Emerging analytical methods to characterize zeolite-based materials. National Science Review 2022, 9 (9) https://doi.org/10.1093/nsr/nwac047
    12. Shichao Peng, Hua Li, Wenjuan Liu, Junyi Yu, Zhaochao Xu, Mao Ye, Zhongmin Liu. Reaction rate enhancement by reducing surface diffusion barriers of guest molecules over ZSM-5 zeolites: a structured illumination microscopy study. Chemical Engineering Journal 2022, 430 , 132760. https://doi.org/10.1016/j.cej.2021.132760
    13. Christian Hess. New advances in using Raman spectroscopy for the characterization of catalysts and catalytic reactions. Chemical Society Reviews 2021, 50 (5) , 3519-3564. https://doi.org/10.1039/D0CS01059F

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