Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography

Joel E. Schmidt; Linqing Peng; Jonathan D. Poplawsky; Bert M. Weckhuysen

doi:10.1002/anie.201712952

Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography

Joel E. Schmidt, Linqing Peng, Jonathan D. Poplawsky, Bert M. Weckhuysen

Materials MicroAnalysis

Research output: Contribution to journal › Review article › peer-review

32 Scopus citations

Abstract

Understanding structure–composition–property relationships in zeolite-based materials is critical to engineering improved solid catalysts. However, this can be difficult to realize as even single zeolite crystals can exhibit heterogeneities spanning several orders of magnitude, with consequences for, for example, reactivity, diffusion as well as stability. Great progress has been made in characterizing these porous solids using tomographic techniques, though each method has an ultimate spatial resolution limitation. Atom probe tomography (APT) is the only technique so far capable of producing 3D compositional reconstructions with sub-nanometer-scale resolution, and has only recently been applied to zeolite-based catalysts. Herein, we discuss the use of APT to study zeolites, including the critical aspects of sample preparation, data collection, assignment of mass spectral peaks including the predominant CO peak, the limitations of spatial resolution for the recovery of crystallographic information, and proper data analysis. All sections are illustrated with examples from recent literature, as well as previously unpublished data and analyses to demonstrate practical strategies to overcome potential pitfalls in applying APT to zeolites, thereby highlighting new insights gained from the APT method.

Original language	English
Pages (from-to)	10422-10435
Number of pages	14
Journal	Angewandte Chemie - International Edition
Volume	57
Issue number	33
DOIs	https://doi.org/10.1002/anie.201712952
State	Published - Aug 13 2018

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 (number 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 from the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement number 702149. L.P. participated in this work at ORNL under the Oak Ridge Science Semester (ORSS) program. 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 (number 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 from the European Union≫s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement number 702149. L.P. participated in this work at ORNL under the Oak Ridge Science Semester (ORSS) program. 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).

Keywords

acidity
atom probe tomography
heterogeneous catalysis
single-atom microscopy
zeolites

Access to Document

10.1002/anie.201712952

Cite this

@article{1f96083b832c4a5783cef6e3e6a9e9e8,

title = "Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography",

abstract = "Understanding structure–composition–property relationships in zeolite-based materials is critical to engineering improved solid catalysts. However, this can be difficult to realize as even single zeolite crystals can exhibit heterogeneities spanning several orders of magnitude, with consequences for, for example, reactivity, diffusion as well as stability. Great progress has been made in characterizing these porous solids using tomographic techniques, though each method has an ultimate spatial resolution limitation. Atom probe tomography (APT) is the only technique so far capable of producing 3D compositional reconstructions with sub-nanometer-scale resolution, and has only recently been applied to zeolite-based catalysts. Herein, we discuss the use of APT to study zeolites, including the critical aspects of sample preparation, data collection, assignment of mass spectral peaks including the predominant CO peak, the limitations of spatial resolution for the recovery of crystallographic information, and proper data analysis. All sections are illustrated with examples from recent literature, as well as previously unpublished data and analyses to demonstrate practical strategies to overcome potential pitfalls in applying APT to zeolites, thereby highlighting new insights gained from the APT method.",

keywords = "acidity, atom probe tomography, heterogeneous catalysis, single-atom microscopy, zeolites",

author = "Schmidt, {Joel E.} and Linqing Peng and Poplawsky, {Jonathan D.} and Weckhuysen, {Bert M.}",

note = "Publisher Copyright: {\textcopyright} 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2018",

month = aug,

day = "13",

doi = "10.1002/anie.201712952",

language = "English",

volume = "57",

pages = "10422--10435",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

publisher = "wiley",

number = "33",

}

TY - JOUR

T1 - Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography

AU - Schmidt, Joel E.

AU - Peng, Linqing

AU - Poplawsky, Jonathan D.

AU - Weckhuysen, Bert M.

PY - 2018/8/13

Y1 - 2018/8/13

N2 - Understanding structure–composition–property relationships in zeolite-based materials is critical to engineering improved solid catalysts. However, this can be difficult to realize as even single zeolite crystals can exhibit heterogeneities spanning several orders of magnitude, with consequences for, for example, reactivity, diffusion as well as stability. Great progress has been made in characterizing these porous solids using tomographic techniques, though each method has an ultimate spatial resolution limitation. Atom probe tomography (APT) is the only technique so far capable of producing 3D compositional reconstructions with sub-nanometer-scale resolution, and has only recently been applied to zeolite-based catalysts. Herein, we discuss the use of APT to study zeolites, including the critical aspects of sample preparation, data collection, assignment of mass spectral peaks including the predominant CO peak, the limitations of spatial resolution for the recovery of crystallographic information, and proper data analysis. All sections are illustrated with examples from recent literature, as well as previously unpublished data and analyses to demonstrate practical strategies to overcome potential pitfalls in applying APT to zeolites, thereby highlighting new insights gained from the APT method.

AB - Understanding structure–composition–property relationships in zeolite-based materials is critical to engineering improved solid catalysts. However, this can be difficult to realize as even single zeolite crystals can exhibit heterogeneities spanning several orders of magnitude, with consequences for, for example, reactivity, diffusion as well as stability. Great progress has been made in characterizing these porous solids using tomographic techniques, though each method has an ultimate spatial resolution limitation. Atom probe tomography (APT) is the only technique so far capable of producing 3D compositional reconstructions with sub-nanometer-scale resolution, and has only recently been applied to zeolite-based catalysts. Herein, we discuss the use of APT to study zeolites, including the critical aspects of sample preparation, data collection, assignment of mass spectral peaks including the predominant CO peak, the limitations of spatial resolution for the recovery of crystallographic information, and proper data analysis. All sections are illustrated with examples from recent literature, as well as previously unpublished data and analyses to demonstrate practical strategies to overcome potential pitfalls in applying APT to zeolites, thereby highlighting new insights gained from the APT method.

KW - acidity

KW - atom probe tomography

KW - heterogeneous catalysis

KW - single-atom microscopy

KW - zeolites

UR - http://www.scopus.com/inward/record.url?scp=85050679247&partnerID=8YFLogxK

U2 - 10.1002/anie.201712952

DO - 10.1002/anie.201712952

M3 - Review article

C2 - 29718553

AN - SCOPUS:85050679247

SN - 1433-7851

VL - 57

SP - 10422

EP - 10435

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 33

ER -

Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this