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Title: Probing the Location and Speciation of Elements in Zeolites with Correlated Atom Probe Tomography and Scanning Transmission X-Ray Microscopy

Abstract

Characterizing materials at nanoscale resolution to provide new insights into structure property performance relationships continues to be a challenging research target due to the inherently low signal from small sample volumes, and is even more difficult for nonconductive materials, such as zeolites. Thus, we present the characterization of a single Cu-exchanged zeolite crystal, namely Cu-SSZ-13, used for NO X reduction in automotive emissions, that was subject to a simulated 135,000-mile aging. By correlating Atom Probe Tomography (APT), a single atom microscopy method, and Scanning Transmission X-ray Microscopy (STXM), which produces high spatial resolution X-ray Absorption Near Edge Spectroscopy (XANES) maps, we show that a spatially non-uniform proportion of the Al was removed from the zeolite framework. Here, the techniques reveal that this degradation is heterogeneous at length scales from micrometers to tens of nanometers, providing complementary insight into the long-term deactivation of this catalyst system.

Authors:
ORCiD logo [1];  [2];  [1]; ORCiD logo [1];  [3];  [3]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [5]; ORCiD logo [1]
  1. Univ. of Utrecht, Utrecht (Netherlands)
  2. Univ. of Utrecht, Utrecht (Netherlands); Nankai Univ., Tianjin (China). Key Lab. of Advanced Energy Materials Chemistry (MOE)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1503580
Grant/Contract Number:  
AC02-76SF00515; 321140
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; scanning transmission; X-ray microscopy; atom probe tomography; zeolites; NOX reduction; chemical imaging

Citation Formats

Schmidt, Joel E., Ye, Xinwei, van Ravenhorst, Ilse K., Oord, Ramon, Shapiro, David A., Yu, Young-Sang, Bare, Simon R., Meirer, Florian, Poplawsky, Jonathan D., and Weckhuysen, Bert M.. Probing the Location and Speciation of Elements in Zeolites with Correlated Atom Probe Tomography and Scanning Transmission X-Ray Microscopy. United States: N. p., 2018. Web. doi:10.1002/cctc.201801378.
Schmidt, Joel E., Ye, Xinwei, van Ravenhorst, Ilse K., Oord, Ramon, Shapiro, David A., Yu, Young-Sang, Bare, Simon R., Meirer, Florian, Poplawsky, Jonathan D., & Weckhuysen, Bert M.. Probing the Location and Speciation of Elements in Zeolites with Correlated Atom Probe Tomography and Scanning Transmission X-Ray Microscopy. United States. doi:10.1002/cctc.201801378.
Schmidt, Joel E., Ye, Xinwei, van Ravenhorst, Ilse K., Oord, Ramon, Shapiro, David A., Yu, Young-Sang, Bare, Simon R., Meirer, Florian, Poplawsky, Jonathan D., and Weckhuysen, Bert M.. Wed . "Probing the Location and Speciation of Elements in Zeolites with Correlated Atom Probe Tomography and Scanning Transmission X-Ray Microscopy". United States. doi:10.1002/cctc.201801378. https://www.osti.gov/servlets/purl/1503580.
@article{osti_1503580,
title = {Probing the Location and Speciation of Elements in Zeolites with Correlated Atom Probe Tomography and Scanning Transmission X-Ray Microscopy},
author = {Schmidt, Joel E. and Ye, Xinwei and van Ravenhorst, Ilse K. and Oord, Ramon and Shapiro, David A. and Yu, Young-Sang and Bare, Simon R. and Meirer, Florian and Poplawsky, Jonathan D. and Weckhuysen, Bert M.},
abstractNote = {Characterizing materials at nanoscale resolution to provide new insights into structure property performance relationships continues to be a challenging research target due to the inherently low signal from small sample volumes, and is even more difficult for nonconductive materials, such as zeolites. Thus, we present the characterization of a single Cu-exchanged zeolite crystal, namely Cu-SSZ-13, used for NOX reduction in automotive emissions, that was subject to a simulated 135,000-mile aging. By correlating Atom Probe Tomography (APT), a single atom microscopy method, and Scanning Transmission X-ray Microscopy (STXM), which produces high spatial resolution X-ray Absorption Near Edge Spectroscopy (XANES) maps, we show that a spatially non-uniform proportion of the Al was removed from the zeolite framework. Here, the techniques reveal that this degradation is heterogeneous at length scales from micrometers to tens of nanometers, providing complementary insight into the long-term deactivation of this catalyst system.},
doi = {10.1002/cctc.201801378},
journal = {ChemCatChem},
issn = {1867-3880},
number = 1,
volume = 11,
place = {United States},
year = {2018},
month = {10}
}

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