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^*

^*Corresponding author for this work

Sub Inorganic Chemistry and Catalysis

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

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
Publication status	Published - 9 Jan 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

Keywords

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

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Schmidt_et_al-2019-ChemCatChemFinal published version, 4.09 MBLicence: CC BY-NC-ND

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

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

year = "2019",

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doi = "10.1002/cctc.201801378",

language = "English",

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AU - Ye, Xinwei

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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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N2 - 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.

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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KW - scanning transmission X-ray microscopy

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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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