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    Revealing Lattice Expansion of Small-Pore Zeolite Catalysts during the Methanol-to-Olefins Process Using Combined Operando X-ray Diffraction and UV–vis Spectroscopy

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    Type
    Article
    Authors
    Goetze, Joris
    Yarulina, Irina
    Gascon, Jorge cc
    Kapteijn, Freek cc
    Weckhuysen, Bert M.
    KAUST Department
    Chemical Engineering Program
    KAUST Catalysis Center (KCC)
    Physical Science and Engineering (PSE) Division
    Date
    2018-02-06
    Online Publication Date
    2018-02-06
    Print Publication Date
    2018-03-02
    Permanent link to this record
    http://hdl.handle.net/10754/627231
    
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    Abstract
    In small-pore zeolite catalysts, where the size of the pores is limited by eight-ring windows, aromatic hydrocarbon pool molecules that are formed inside the zeolite during the Methanol-to-Olefins (MTO) process cannot exit the pores and are retained inside the catalyst. Hydrocarbon species whose size is comparable to the size of the zeolite cage can cause the zeolite lattice to expand during the MTO process. In this work, the formation of retained hydrocarbon pool species during MTO at a reaction temperature of 400 °C was followed using operando UV–vis spectroscopy. During the same experiment, using operando X-ray Diffraction (XRD), the expansion of the zeolite framework was assessed, and the activity of the catalyst was measured using online gas chromatography (GC). Three different small-pore zeolite frameworks, i.e., CHA, DDR, and LEV, were compared. It was shown using operando XRD that the formation of retained aromatic species causes the zeolite lattice of all three frameworks to expand. Because of the differences in the zeolite framework dimensions, the nature of the retained hydrocarbons as measured by operando UV–vis spectroscopy is different for each of the three zeolite frameworks. Consequently, the magnitude and direction of the zeolite lattice expansion as measured by operando XRD also depends on the specific combination of the hydrocarbon species and the zeolite framework. The catalyst with the CHA framework, i.e., H-SSZ-13, showed the biggest expansion: 0.9% in the direction along the c-axis of the zeolite lattice. For all three zeolite frameworks, based on the combination of operando XRD and operando UV–vis spectroscopy, the hydrocarbon species that are likely to cause the expansion of the zeolite cages are presented; methylated naphthalene and pyrene in CHA, 1-methylnaphthalene and phenalene in DDR, and methylated benzene and naphthalene in LEV. Filling of the zeolite cages and, as a consequence, the zeolite lattice expansion causes the deactivation of these small-pore zeolite catalysts during the MTO process.
    Citation
    Goetze J, Yarulina I, Gascon J, Kapteijn F, Weckhuysen BM (2018) Revealing Lattice Expansion of Small-Pore Zeolite Catalysts during the Methanol-to-Olefins Process Using Combined Operando X-ray Diffraction and UV–vis Spectroscopy. ACS Catalysis 8: 2060–2070. Available: http://dx.doi.org/10.1021/acscatal.7b04129.
    Sponsors
    This research received funding from The Netherlands Organisation for Scientific Research (NWO) in the framework of the TASC Technology Area “Syngas, a Switch to Flexible New Feedstock for the Chemical Industry (TA-Syngas)”.
    Publisher
    American Chemical Society (ACS)
    Journal
    ACS Catalysis
    DOI
    10.1021/acscatal.7b04129
    Additional Links
    https://pubs.acs.org/doi/10.1021/acscatal.7b04129
    ae974a485f413a2113503eed53cd6c53
    10.1021/acscatal.7b04129
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Engineering Program; KAUST Catalysis Center (KCC)

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