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

Joel E. Schmidt; Xinwei Ye; Ilse K. van Ravenhorst; Ramon Oord; David A. Shapiro; Young Sang Yu; Simon R. Bare; Florian Meirer; Jonathan D. Poplawsky; Bert M. Weckhuysen

doi:10.1002/cctc.201801378

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

Joel E. Schmidt, Xinwei Ye, Ilse K. van Ravenhorst, Ramon Oord, David A. Shapiro, Young Sang Yu, Simon R. Bare, Florian Meirer, Jonathan D. Poplawsky, Bert M. Weckhuysen

Materials MicroAnalysis

Research output: Contribution to journal › Article › peer-review

18 Scopus citations

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. Herein, 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. 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.

Original language	English
Pages (from-to)	488-494
Number of pages	7
Journal	ChemCatChem
Volume	11
Issue number	1
DOIs	https://doi.org/10.1002/cctc.201801378
State	Published - Jan 9 2019

Funding

This work is supported by the NWO Gravitation program, Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), and a European Research Council (ERC) Advanced Grant (No. 321140). The APT measurements were conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. J.S. has received funding under the Marie Sklodow-ska-Curie Grant Agreement No. 702149. X.Y. acknowledges support from China Scholarship Council (CSC). This research used resources of the Advanced Light Source, which is a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. This manuscript has been authored by UT-Battelle, LLC under contract number DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http:// energy.gov/downloads/doe-public-access-plan). This work is supported by the NWO Gravitation program, Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), and a European Research Council (ERC) Advanced Grant (No. 321140). The APT measurements were conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. J.S. has received funding under the Marie Sklodowska-Curie Grant Agreement No. 702149. X.Y. acknowledges support from China Scholarship Council (CSC). This research used resources of the Advanced Light Source, which is a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. This manuscript has been authored by UT-Battelle, LLC under contract number DE- AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

Funders	Funder number
DOE Office of Science
DOE Public Access Plan
MCEC
Marie Sklodow-ska-Curie
Netherlands Center for Multiscale Catalytic Energy Conversion
United States Government
U.S. Department of Energy
Horizon 2020 Framework Programme	321140, 702149
European Research Council
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
China Scholarship Council	DE-AC05-00OR22725

Keywords

NO reduction
atom probe tomography
chemical imaging
scanning transmission X-ray microscopy
zeolites

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10.1002/cctc.201801378

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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. Herein, 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. 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.",

keywords = "NO reduction, atom probe tomography, chemical imaging, scanning transmission X-ray microscopy, zeolites",

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AU - Oord, Ramon

AU - Shapiro, David A.

AU - Yu, Young Sang

AU - Bare, Simon R.

AU - Meirer, Florian

AU - Poplawsky, Jonathan D.

AU - Weckhuysen, Bert M.

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AB - 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. Herein, 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. 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.

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

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