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

Daniel E. Perea, Ilke Arslan, Jia Liu, Zoran Ristanović, Libor Kovarik, Bruce W. Arey, Johannes A. Lercher, Simon R. Bare () and Bert M. Weckhuysen ()
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Daniel E. Perea: Pacific Northwest National Laboratory, Environmental Molecular Science Laboratory
Ilke Arslan: Pacific Northwest National Laboratory, Institute for Integrated Catalysis
Jia Liu: Pacific Northwest National Laboratory, Environmental Molecular Science Laboratory
Zoran Ristanović: Faculty of Science, Debye Institute for Nanomaterials Science, Utrecht University
Libor Kovarik: Pacific Northwest National Laboratory, Environmental Molecular Science Laboratory
Bruce W. Arey: Pacific Northwest National Laboratory, Environmental Molecular Science Laboratory
Johannes A. Lercher: Pacific Northwest National Laboratory, Institute for Integrated Catalysis
Simon R. Bare: UOP LLC, a Honeywell Company
Bert M. Weckhuysen: Faculty of Science, Debye Institute for Nanomaterials Science, Utrecht University

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: 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. 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.

Date: 2015
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DOI: 10.1038/ncomms8589

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