Micro‐ and Nanoscale Heterogeneities in Zeolite Beta as Measured by Atom Probe Tomography and Confocal Fluorescence Microscopy

Author:

van Vreeswijk Sophie H.1,Parker Luke A.12,Maris J. J. Erik1,Poplawsky Jonathan D.3,Weckhuysen Bert M.1ORCID

Affiliation:

1. Inorganic Chemistry and Catalysis Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterial Science Utrecht University Universiteitsweg 99 3584 CG Utrecht The Netherlands

2. Current address: TNO Environmental Modelling, Sensing and Analysis Princetonlaan 6 3584 CB Utrecht The Netherlands

3. Center for Nanophase Materials Sciences Oak Ridge National Laboratory Oak Ridge TN 37831 USA

Abstract

AbstractMicro‐ and nanoscale information on the activating and deactivating coking behaviour of zeolite catalyst materials increases our current understanding of many industrially applied processes, such as the methanol‐to‐hydrocarbon (MTH) reaction. Atom probe tomography (APT) was used to reveal the link between framework and coke elemental distributions in 3D with sub‐nanometre resolution. APT revealed 10–20 nanometre‐sized Al‐rich regions and short‐range ordering (within nanometres) between Al atoms. With confocal fluorescence microscopy, it was found that the morphology of the zeolite crystal as well as the secondary mesoporous structures have a great effect on the microscale coke distribution throughout individual zeolite crystals over time. Additionally, a nanoscale heterogeneous distribution of carbon as residue from the MTH reaction was determined with carbon‐rich areas of tens of nanometres within the zeolite crystals. Lastly, a short length‐scale affinity between C and Al atoms, as revealed by APT, indicates the formation of carbon‐containing molecules next to the acidic sites in the zeolite.

Funder

Ministry of Higher Education and Scientific Research

Army Research Office

Publisher

Wiley

Subject

Physical and Theoretical Chemistry,Atomic and Molecular Physics, and Optics

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