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Title: Steam‐Induced Coarsening of Single‐Unit‐Cell MFI Zeolite Nanosheets and Its Effect on External Surface Brønsted Acid Catalysis

Abstract

Abstract Commonly used methods to assess crystallinity, micro‐/mesoporosity, Brønsted acid site density and distribution (in micro‐ vs. mesopores), and catalytic activity suggest nearly invariant structure and function for aluminosilicate zeolite MFI two‐dimensional nanosheets before and after superheated steam treatment. Yet, pronounced reaction rate decrease for benzyl alcohol alkylation with mesitylene, a reaction that cannot take place in the zeolite micropores, is observed. Transmission electron microscopy images reveal pronounced changes in nanosheet thickness, aspect ratio and roughness indicating that nanosheet coarsening and the associated changes in the external (mesoporous) surface structure are responsible for the changes in the external surface catalytic activity. Superheated steam treatment of hierarchical zeolites can be used to alter nanosheet morphology and regulate external surface catalytic activity while preserving micro‐ and mesoporosity, and micropore reaction rates.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [3];  [1];  [2];  [4]; ORCiD logo [5]
  1. Department of Chemical Engineering and Materials Science University of Minnesota 421 Washington Avenue SE Minneapolis MN 55455 USA
  2. Peter A. Rock Thermochemistry Laboratory NEAT-ORU University of California Davis Davis CA 95616 USA
  3. Department of Chemical Engineering Khalifa University of Science and Technology Habshan Building, Sas Al Nakhl Campus Abu Dhabi United Arab Emirates
  4. Department of Diagnostic and Biological Sciences University of Minnesota 515 Delaware St SE Minneapolis MN 55455 USA, Characterization Facility University of Minnesota 312 Church St Minneapolis MN 55455 USA
  5. Department of Chemical Engineering and Materials Science University of Minnesota 421 Washington Avenue SE Minneapolis MN 55455 USA, Department of Chemical and Biomolecular Engineering and Institute for NanoBioTechnology Johns Hopkins University 3400 N. Charles Street Baltimore MD 21218 USA, Applied Physics Laboratory Johns Hopkins University 11100 Johns Hopkins Road Laurel MD 20723 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1631505
Grant/Contract Number:  
SC0001004
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Name: Angewandte Chemie Journal Volume: 132 Journal Issue: 24; Journal ID: ISSN 0044-8249
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Guefrachi, Yasmine, Sharma, Geetu, Xu, Dandan, Kumar, Gaurav, Vinter, Katherine P., Abdelrahman, Omar A., Li, Xinyu, Alhassan, Saeed, Dauenhauer, Paul J., Navrotsky, Alexandra, Zhang, Wei, and Tsapatsis, Michael. Steam‐Induced Coarsening of Single‐Unit‐Cell MFI Zeolite Nanosheets and Its Effect on External Surface Brønsted Acid Catalysis. Germany: N. p., 2020. Web. doi:10.1002/ange.202000395.
Guefrachi, Yasmine, Sharma, Geetu, Xu, Dandan, Kumar, Gaurav, Vinter, Katherine P., Abdelrahman, Omar A., Li, Xinyu, Alhassan, Saeed, Dauenhauer, Paul J., Navrotsky, Alexandra, Zhang, Wei, & Tsapatsis, Michael. Steam‐Induced Coarsening of Single‐Unit‐Cell MFI Zeolite Nanosheets and Its Effect on External Surface Brønsted Acid Catalysis. Germany. https://doi.org/10.1002/ange.202000395
Guefrachi, Yasmine, Sharma, Geetu, Xu, Dandan, Kumar, Gaurav, Vinter, Katherine P., Abdelrahman, Omar A., Li, Xinyu, Alhassan, Saeed, Dauenhauer, Paul J., Navrotsky, Alexandra, Zhang, Wei, and Tsapatsis, Michael. Thu . "Steam‐Induced Coarsening of Single‐Unit‐Cell MFI Zeolite Nanosheets and Its Effect on External Surface Brønsted Acid Catalysis". Germany. https://doi.org/10.1002/ange.202000395.
@article{osti_1631505,
title = {Steam‐Induced Coarsening of Single‐Unit‐Cell MFI Zeolite Nanosheets and Its Effect on External Surface Brønsted Acid Catalysis},
author = {Guefrachi, Yasmine and Sharma, Geetu and Xu, Dandan and Kumar, Gaurav and Vinter, Katherine P. and Abdelrahman, Omar A. and Li, Xinyu and Alhassan, Saeed and Dauenhauer, Paul J. and Navrotsky, Alexandra and Zhang, Wei and Tsapatsis, Michael},
abstractNote = {Abstract Commonly used methods to assess crystallinity, micro‐/mesoporosity, Brønsted acid site density and distribution (in micro‐ vs. mesopores), and catalytic activity suggest nearly invariant structure and function for aluminosilicate zeolite MFI two‐dimensional nanosheets before and after superheated steam treatment. Yet, pronounced reaction rate decrease for benzyl alcohol alkylation with mesitylene, a reaction that cannot take place in the zeolite micropores, is observed. Transmission electron microscopy images reveal pronounced changes in nanosheet thickness, aspect ratio and roughness indicating that nanosheet coarsening and the associated changes in the external (mesoporous) surface structure are responsible for the changes in the external surface catalytic activity. Superheated steam treatment of hierarchical zeolites can be used to alter nanosheet morphology and regulate external surface catalytic activity while preserving micro‐ and mesoporosity, and micropore reaction rates.},
doi = {10.1002/ange.202000395},
journal = {Angewandte Chemie},
number = 24,
volume = 132,
place = {Germany},
year = {Thu Apr 02 00:00:00 EDT 2020},
month = {Thu Apr 02 00:00:00 EDT 2020}
}

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