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dc.contributor.authorGoetze, Joris
dc.contributor.authorYarulina, Irina
dc.contributor.authorGascon, Jorge
dc.contributor.authorKapteijn, Freek
dc.contributor.authorWeckhuysen, Bert M.
dc.date.accessioned2018-03-06T06:50:09Z
dc.date.available2018-03-06T06:50:09Z
dc.date.issued2018-02-06
dc.identifier.citationGoetze 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.
dc.identifier.issn2155-5435
dc.identifier.issn2155-5435
dc.identifier.doi10.1021/acscatal.7b04129
dc.identifier.urihttp://hdl.handle.net/10754/627231
dc.description.abstractIn 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.
dc.description.sponsorshipThis 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)”.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/acscatal.7b04129
dc.rightsThis is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License, which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
dc.rights.urihttp://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html
dc.subjectdeactivation
dc.subjectlattice expansion
dc.subjectMethanol-to-Olefins
dc.subjectoperando
dc.subjectRietveld refinement
dc.subjectUV−vis spectroscopy
dc.subjectX-ray diffraction
dc.subjectzeolites
dc.titleRevealing Lattice Expansion of Small-Pore Zeolite Catalysts during the Methanol-to-Olefins Process Using Combined Operando X-ray Diffraction and UV–vis Spectroscopy
dc.typeArticle
dc.contributor.departmentChemical Engineering Program
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalACS Catalysis
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionInorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands
dc.contributor.institutionCatalysis Engineering, Chemical Engineering Department, Delft University of Technology, Van der Maasweg 9, 2629 HZ Delft, The Netherlands
kaust.personYarulina, Irina
kaust.personGascon, Jorge
refterms.dateFOA2018-06-14T05:02:09Z
dc.date.published-online2018-02-06
dc.date.published-print2018-03-02


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