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Title: Coke formation in a zeolite crystal during the methanol-to-hydrocarbons reaction as studied with atom probe tomography

Abstract

Understanding the formation of carbon deposits in zeolites is vital to developing new, superior materials for various applications, including oil and gas conversion processes. Herein, atom probe tomography (APT) has been used to spatially resolve the 3D compositional changes at the sub-nm length scale in a single zeolite ZSM-5 crystal, which has been partially deactivated by the methanol-to-hydrocarbons reaction using 13C-labeled methanol. The results reveal the formation of coke in agglomerates that span length scales from tens of nanometers to atomic clusters with a median size of 30–60 13C atoms. These clusters correlate with local increases in Brønsted acid site density, demonstrating that the formation of the first deactivating coke precursor molecules occurs in nanoscopic regions enriched in aluminum. Here, this nanoscale correlation underscores the importance of carefully engineering materials to suppress detrimental coke formation.

Authors:
 [1];  [2];  [2];  [1];  [1];  [1];  [1];  [3];  [1]
  1. Utrecht Univ., Utrecht (Netherlands)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1324189
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 37; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; zeolites; atom probe tomography; carbon deposits; Al zoning; methanol to hydrocarbons

Citation Formats

Schmidt, Joel E., Poplawsky, Jonathan D., Mazumder, Baishakhi, Attila, Özgün, Fu, Donglong, de Winter, D. A. Matthijs, Meirer, Florian, Bare, Simon R., and Weckhuysen, Bert M. Coke formation in a zeolite crystal during the methanol-to-hydrocarbons reaction as studied with atom probe tomography. United States: N. p., 2016. Web. doi:10.1002/anie.201606099.
Schmidt, Joel E., Poplawsky, Jonathan D., Mazumder, Baishakhi, Attila, Özgün, Fu, Donglong, de Winter, D. A. Matthijs, Meirer, Florian, Bare, Simon R., & Weckhuysen, Bert M. Coke formation in a zeolite crystal during the methanol-to-hydrocarbons reaction as studied with atom probe tomography. United States. doi:10.1002/anie.201606099.
Schmidt, Joel E., Poplawsky, Jonathan D., Mazumder, Baishakhi, Attila, Özgün, Fu, Donglong, de Winter, D. A. Matthijs, Meirer, Florian, Bare, Simon R., and Weckhuysen, Bert M. Wed . "Coke formation in a zeolite crystal during the methanol-to-hydrocarbons reaction as studied with atom probe tomography". United States. doi:10.1002/anie.201606099. https://www.osti.gov/servlets/purl/1324189.
@article{osti_1324189,
title = {Coke formation in a zeolite crystal during the methanol-to-hydrocarbons reaction as studied with atom probe tomography},
author = {Schmidt, Joel E. and Poplawsky, Jonathan D. and Mazumder, Baishakhi and Attila, Özgün and Fu, Donglong and de Winter, D. A. Matthijs and Meirer, Florian and Bare, Simon R. and Weckhuysen, Bert M.},
abstractNote = {Understanding the formation of carbon deposits in zeolites is vital to developing new, superior materials for various applications, including oil and gas conversion processes. Herein, atom probe tomography (APT) has been used to spatially resolve the 3D compositional changes at the sub-nm length scale in a single zeolite ZSM-5 crystal, which has been partially deactivated by the methanol-to-hydrocarbons reaction using 13C-labeled methanol. The results reveal the formation of coke in agglomerates that span length scales from tens of nanometers to atomic clusters with a median size of 30–60 13C atoms. These clusters correlate with local increases in Brønsted acid site density, demonstrating that the formation of the first deactivating coke precursor molecules occurs in nanoscopic regions enriched in aluminum. Here, this nanoscale correlation underscores the importance of carefully engineering materials to suppress detrimental coke formation.},
doi = {10.1002/anie.201606099},
journal = {Angewandte Chemie (International Edition)},
number = 37,
volume = 55,
place = {United States},
year = {Wed Aug 03 00:00:00 EDT 2016},
month = {Wed Aug 03 00:00:00 EDT 2016}
}

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Cited by: 9 works
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