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

Daniel E. Perea; Ilke Arslan; Jia Liu; Zoran Ristanovic; Libor Kovarik; Bruce W. Arey; Johannes A. Lercher; Simon R. Bare; Bert M. Weckhuysen

doi:10.1038/ncomms8589

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

Daniel E. Perea
, Ilke Arslan
, Jia Liu
, Zoran Ristanovic
, Libor Kovarik
, Bruce W. Arey
, Johannes A. Lercher
, Simon R. Bare^*
, Bert M. Weckhuysen

^*Corresponding author for this work

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

Abstract

Zeolite catalysis is determined by a combination of pore architecture and Bronsted acidity. As Bronsted 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. 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.

Original language	English
Article number	7589
Number of pages	8
Journal	Nature Communications [E]
Volume	6
DOIs	https://doi.org/10.1038/ncomms8589
Publication status	Published - Jul 2015

Funding

The APT experiments in this study were performed under a science theme user proposal at EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. I. A. acknowledges support through the LDRD programme at PNNL. PNNL is operated by Battelle for the U.S. Department of Energy under contract DE-AC05-76RL01830. B.M.W. acknowledges financial support from the Netherlands Organisation for Scientific Research (NWO) Gravitation Program (Netherlands Center for Multiscale Catalytic Energy Conversion, MCEC) and a TOP NWO-CW Grant, as well as a European Research Council (ERC) Advanced Grant (321140). We acknowledge Machteld Mertens (ExxonMobil) for making the zeolite ZSM-5 crystals.

Keywords

MQ MAS NMR
ZSM-5 CRYSTALS
LOCAL-STRUCTURE
AL-27 MAS
ALK-EDGE
T-SITES
COORDINATION
ACIDITY
SPECTROSCOPY
BETA

Access to Document

10.1038/ncomms8589

ncomms8589Final published version, 2.17 MB

Cite this

@article{bf951ba0c53d4b05a5dafa9eab14be0c,

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 Bronsted acidity. As Bronsted 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. 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.",

keywords = "MQ MAS NMR, ZSM-5 CRYSTALS, LOCAL-STRUCTURE, AL-27 MAS, ALK-EDGE, T-SITES, COORDINATION, ACIDITY, SPECTROSCOPY, BETA",

author = "Perea, \{Daniel E.\} and Ilke Arslan and Jia Liu and Zoran Ristanovic and Libor Kovarik and Arey, \{Bruce W.\} and Lercher, \{Johannes A.\} and Bare, \{Simon R.\} and Weckhuysen, \{Bert M.\}",

year = "2015",

month = jul,

doi = "10.1038/ncomms8589",

language = "English",

volume = "6",

journal = "Nature Communications [E]",

issn = "2041-1723",

publisher = "Nature Research",

}

TY - JOUR

T1 - Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography

AU - Perea, Daniel E.

AU - Arslan, Ilke

AU - Liu, Jia

AU - Ristanovic, Zoran

AU - Kovarik, Libor

AU - Arey, Bruce W.

AU - Lercher, Johannes A.

AU - Bare, Simon R.

AU - Weckhuysen, Bert M.

PY - 2015/7

Y1 - 2015/7

N2 - Zeolite catalysis is determined by a combination of pore architecture and Bronsted acidity. As Bronsted 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. 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.

AB - Zeolite catalysis is determined by a combination of pore architecture and Bronsted acidity. As Bronsted 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. 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.

KW - MQ MAS NMR

KW - ZSM-5 CRYSTALS

KW - LOCAL-STRUCTURE

KW - AL-27 MAS

KW - ALK-EDGE

KW - T-SITES

KW - COORDINATION

KW - ACIDITY

KW - SPECTROSCOPY

KW - BETA

U2 - 10.1038/ncomms8589

DO - 10.1038/ncomms8589

M3 - Article

SN - 2041-1723

VL - 6

JO - Nature Communications [E]

JF - Nature Communications [E]

M1 - 7589

ER -

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

Abstract

Funding

Keywords

Access to Document

Fingerprint

Cite this