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

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

doi:10.1002/anie.202000395

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

Journal Article · Sun Mar 01 00:00:00 EST 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202000395· OSTI ID:1767524

Guefrachi, Yasmine ^[1]; Sharma, Geetu ^[2]; Xu, Dandan ^[3]; Kumar, Gaurav ^[3]; Vinter, Katherine P. ^[3]; Abdelrahman, Omar A. ^[3]; Li, Xinyu ^[3]; Alhassan, Saeed ^[4]; Dauenhauer, Paul J. ^[3]; Navrotsky, Alexandra ^[2]; Zhang, Wei ^[3]; ^[5]

Univ. of Minnesota, Minneapolis, MN (United States); OSTI
Univ. of California, Davis CA (United States)
Univ. of Minnesota, Minneapolis, MN (United States)
Khalifa Univ. of Science and Technology, Abu Dhabi (United Arab Emirates)
Univ. of Minnesota, Minneapolis, MN (United States); Johns Hopkins Univ., Baltimore, MD (United States)

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. Finally, 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.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI); Univ. of Delaware, Newark, DE (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001004

OSTI ID:: 1767524

Alternate ID(s):: OSTI ID: 1631759

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 24 Vol. 59; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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