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Title: Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography

Abstract

Zeolite catalysis is determined by a combination of pore architecture and Brønsted acidity. As Brønsted acid sites are formed by the substitution of AlO4 for SiO4 tetrahedra, it is of utmost importance to have information on the number as well as the location and neighbouring sites of framework aluminium. Unfortunately, such detailed information has not yet been obtained, mainly due to the lack of suitable characterization methods. Here we report, using the powerful atomic-scale analysis technique known as atom probe tomography, the quantitative spatial distribution of individual aluminium atoms, including their three-dimensional extent of segregation. Ultimately, using a nearest-neighbour statistical analysis, we precisely determine the short-range distribution of aluminium over the different T-sites and determine the most probable Al–Al neighbouring distance within parent and steamed ZSM-5 crystals, as well as assess the long-range redistribution of aluminium upon zeolite steaming.

Authors:
 [1];  [2];  [1];  [3];  [1];  [1];  [4];  [5];  [3]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis
  3. Univ. of Utrecht (Netherlands)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis; Technische Univ. of Munich, Garching (Germany)
  5. UOP LLC, Des Plaines, IL (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1260735
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Perea, Daniel E., Arslan, Ilke, Liu, Jia, Ristanović, Zoran, Kovarik, Libor, Arey, Bruce W., Lercher, Johannes A., Bare, Simon R., and Weckhuysen, Bert M. Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography. United States: N. p., 2015. Web. doi:10.1038/ncomms8589.
Perea, Daniel E., Arslan, Ilke, Liu, Jia, Ristanović, Zoran, Kovarik, Libor, Arey, Bruce W., Lercher, Johannes A., Bare, Simon R., & Weckhuysen, Bert M. Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography. United States. https://doi.org/10.1038/ncomms8589
Perea, Daniel E., Arslan, Ilke, Liu, Jia, Ristanović, Zoran, Kovarik, Libor, Arey, Bruce W., Lercher, Johannes A., Bare, Simon R., and Weckhuysen, Bert M. 2015. "Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography". United States. https://doi.org/10.1038/ncomms8589. https://www.osti.gov/servlets/purl/1260735.
@article{osti_1260735,
title = {Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography},
author = {Perea, Daniel E. and Arslan, Ilke and Liu, Jia and Ristanović, Zoran and Kovarik, Libor and Arey, Bruce W. and Lercher, Johannes A. and Bare, Simon R. and Weckhuysen, Bert M.},
abstractNote = {Zeolite catalysis is determined by a combination of pore architecture and Brønsted acidity. As Brønsted acid sites are formed by the substitution of AlO4 for SiO4 tetrahedra, it is of utmost importance to have information on the number as well as the location and neighbouring sites of framework aluminium. Unfortunately, such detailed information has not yet been obtained, mainly due to the lack of suitable characterization methods. Here we report, using the powerful atomic-scale analysis technique known as atom probe tomography, the quantitative spatial distribution of individual aluminium atoms, including their three-dimensional extent of segregation. Ultimately, using a nearest-neighbour statistical analysis, we precisely determine the short-range distribution of aluminium over the different T-sites and determine the most probable Al–Al neighbouring distance within parent and steamed ZSM-5 crystals, as well as assess the long-range redistribution of aluminium upon zeolite steaming.},
doi = {10.1038/ncomms8589},
url = {https://www.osti.gov/biblio/1260735}, journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 6,
place = {United States},
year = {Thu Jul 02 00:00:00 EDT 2015},
month = {Thu Jul 02 00:00:00 EDT 2015}
}

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Cited by: 118 works
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Works referenced in this record:

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  • van Bokhoven, Jeroen A.; van der Eerden, Ad M. J.; Koningsberger, Diek C.
  • Journal of the American Chemical Society, Vol. 125, Issue 24
  • https://doi.org/10.1021/ja0292905

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Works referencing / citing this record:

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Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography
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Micro-spectroscopy of HKUST-1 metal–organic framework crystals loaded with tetracyanoquinodimethane: effects of water on host–guest chemistry and electrical conductivity
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Acidity enhancement through synergy of penta- and tetra-coordinated aluminum species in amorphous silica networks
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Mechanistic insights into aqueous phase propanol dehydration in H-ZSM-5 zeolite
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Advances in atom probe tomography instrumentation: Implications for materials research
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X-ray Excited Optical Fluorescence and Diffraction Imaging of Reactivity and Crystallinity in a Zeolite Crystal: Crystallography and Molecular Spectroscopy in One
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Decarboxylation of stearic acid over Ni/MOR catalysts
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Nanoscale Chemical Imaging of Zeolites Using Atom Probe Tomography
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Conversion of Palmitic Acid Over Bi-functional Ni/ZSM-5 Catalyst: Effect of Stoichiometric Ni/Al Molar Ratio
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Nanoscale tomography reveals the deactivation of automotive copper-exchanged zeolite catalysts
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Atom Probe Tomography for Catalysis Applications: A Review
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Reversible and Site-Dependent Proton-Transfer in Zeolites Uncovered at the Single-Molecule Level
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In-line three-dimensional holography of nanocrystalline objects at atomic resolution
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Coke Formation in a Zeolite Crystal During the Methanol-to-Hydrocarbons Reaction as Studied with Atom Probe Tomography
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Defining Aluminum-Zoning during Synthesis of ZSM-5 Zeolites
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Characterization of Metal‐zeolite Composite Catalysts: Determining the Environment of the Active Phase
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Acidity enhancement through synergy of penta- and tetra-coordinated aluminum species in amorphous silica networks
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An environmental transfer hub for multimodal atom probe tomography
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In-line three-dimensional holography of nanocrystalline objects at atomic resolution
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Coke Formation in a Zeolite Crystal During the Methanol-to-Hydrocarbons Reaction as Studied with Atom Probe Tomography
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Coke Formation in a Zeolite Crystal During the Methanol-to-Hydrocarbons Reaction as Studied with Atom Probe Tomography
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