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Title: Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts

Abstract

The nanoscale compositional mapping of fresh HZSM-5 catalyst synthesized using hydrothermal process as well as after just steaming and after ethanol conversion reaction for 72 hours at realistic catalytic conditions was investigated using atom probe tomography. Atom probe tomography permitted direct atomic scale imaging of non-uniform distribution of Al within the HZSM-5 as well as for the first time image the hydrocarbon coking after ethanol reaction. Clear evidences for existence of multiple C-H molecular species which appear to aggregate as clusters within the pores of spent HZSM-5 catalyst materials is provided. Furthermore, these results provide evidence for the ability of atom probe tomography, a powerful 3D characterization tool in interrogating the atomic scale chemistry of zeolite catalyst materials at industrially relevant catalytic conditions.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1334859
Report Number(s):
PNNL-SA-113562
Journal ID: ISSN 2045-2322; BM0102060
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Devaraj, Arun, Vijayakumar, Murugesan, Bao, Jie, Guo, Mond F., Derewinski, Miroslaw A., Xu, Zhijie, Gray, Michel J., Prodinger, Sebastian, and Ramasamy, Karthikeyan K. Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts. United States: N. p., 2016. Web. doi:10.1038/srep37586.
Devaraj, Arun, Vijayakumar, Murugesan, Bao, Jie, Guo, Mond F., Derewinski, Miroslaw A., Xu, Zhijie, Gray, Michel J., Prodinger, Sebastian, & Ramasamy, Karthikeyan K. Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts. United States. doi:10.1038/srep37586.
Devaraj, Arun, Vijayakumar, Murugesan, Bao, Jie, Guo, Mond F., Derewinski, Miroslaw A., Xu, Zhijie, Gray, Michel J., Prodinger, Sebastian, and Ramasamy, Karthikeyan K. Wed . "Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts". United States. doi:10.1038/srep37586. https://www.osti.gov/servlets/purl/1334859.
@article{osti_1334859,
title = {Discerning the Location and Nature of Coke Deposition from Surface to Bulk of Spent Zeolite Catalysts},
author = {Devaraj, Arun and Vijayakumar, Murugesan and Bao, Jie and Guo, Mond F. and Derewinski, Miroslaw A. and Xu, Zhijie and Gray, Michel J. and Prodinger, Sebastian and Ramasamy, Karthikeyan K.},
abstractNote = {The nanoscale compositional mapping of fresh HZSM-5 catalyst synthesized using hydrothermal process as well as after just steaming and after ethanol conversion reaction for 72 hours at realistic catalytic conditions was investigated using atom probe tomography. Atom probe tomography permitted direct atomic scale imaging of non-uniform distribution of Al within the HZSM-5 as well as for the first time image the hydrocarbon coking after ethanol reaction. Clear evidences for existence of multiple C-H molecular species which appear to aggregate as clusters within the pores of spent HZSM-5 catalyst materials is provided. Furthermore, these results provide evidence for the ability of atom probe tomography, a powerful 3D characterization tool in interrogating the atomic scale chemistry of zeolite catalyst materials at industrially relevant catalytic conditions.},
doi = {10.1038/srep37586},
journal = {Scientific Reports},
number = ,
volume = 6,
place = {United States},
year = {Wed Nov 23 00:00:00 EST 2016},
month = {Wed Nov 23 00:00:00 EST 2016}
}

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Works referenced in this record:

Conversion of Methanol to Hydrocarbons: How Zeolite Cavity and Pore Size Controls Product Selectivity
journal, April 2012

  • Olsbye, Unni; Svelle, Stian; Bjørgen, Morten
  • Angewandte Chemie International Edition, Vol. 51, Issue 24, p. 5810-5831
  • DOI: 10.1002/anie.201103657