3-D X-ray Nanotomography Reveals Different Carbon Deposition Mechanisms in a Single Catalyst Particle
Veselý, Martin; Valadian, Roozbeh; Merten Lohse, Leon; Toepperwien, Mareike; Spiers, Kathryn; Garrevoet, Jan; Vogt, Eelco T. C.; Salditt, Tim; Weckhuysen, Bert M.; Meirer, Florian
(2021) ChemCatChem, volume 13, issue 10, pp. 2494 - 2507
(Article)
Abstract
Catalyst deactivation involves a complex interplay of processes taking place at different length and time scales. Understanding this phenomenon is one of the grand challenges in solid catalyst characterization. A process contributing to deactivation is carbon deposition (i.?e., coking), which reduces catalyst activity by limiting diffusion and blocking active sites.
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However, characterizing coke formation and its effects remains challenging as it involves both the organic and inorganic phase of the catalytic process and length scales from the atomic scale to the scale of the catalyst body. Here we present a combination of hard X-ray imaging techniques able to visualize in 3-D the distribution, effect and nature of carbon deposits in the macro-pore space of an entire industrially used catalyst particle. Our findings provide direct evidence for coke promoting effects of metal poisons, pore clogging by coke, and a correlation between carbon nature and its location. These results provide a better understanding of the coking process, its relation to catalyst deactivation and new insights into the efficiency of the industrial scale process of fluid catalytic cracking.
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Keywords: Fluid catalytic cracking, X-ray holotomography, carbon deposits, individual catalyst particle, pore network, Catalysis, Physical and Theoretical Chemistry, Organic Chemistry, Inorganic Chemistry
ISSN: 1867-3880
Publisher: Wiley - VCH Verlag GmbH & CO. KGaA
Note: Funding Information: We thank Dr. Marianna Gambino (Utrecht University, UU) and Dr. Matthias Filez (UU) for fruitful discussions, and Dr. Michael Sprung (DESY) for assistance during the experiments at DESY. Dr. Thomas Gaudisson (UU) is acknowledged for designing the calcination chamber. Dr. Andrei V. Petukhov (UU) is acknowledged for helping with the interpretation of the SAXS data. The work is supported by a Netherlands Organization for Scientific Research (NWO) VIDI Grant No. 723.015.007 (to FM) as well as by a NWO Gravitation program, Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC) (to BMW). Parts of this research were carried out at a ?beamline/facility? at DESY, a member of the Helmholtz Association (HGF). The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. This research was supported in part through the Maxwell computational resources operated at Deutsches Elektronen-Synchrotron (DESY), Hamburg, Germany. Funding Information: We thank Dr. Marianna Gambino (Utrecht University, UU) and Dr. Matthias Filez (UU) for fruitful discussions, and Dr. Michael Sprung (DESY) for assistance during the experiments at DESY. Dr. Thomas Gaudisson (UU) is acknowledged for designing the calcination chamber. Dr. Andrei V. Petukhov (UU) is acknowledged for helping with the interpretation of the SAXS data. The work is supported by a Netherlands Organization for Scientific Research (NWO) VIDI Grant No. 723.015.007 (to FM) as well as by a NWO Gravitation program, Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC) (to BMW). Parts of this research were carried out at a “beamline/facility” at DESY, a member of the Helmholtz Association (HGF). The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. This research was supported in part through the Maxwell computational resources operated at Deutsches Elektronen‐Synchrotron (DESY), Hamburg, Germany. Publisher Copyright: © 2021 The Authors. ChemCatChem published by Wiley-VCH GmbH
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