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dc.contributor.authorVollmer, Ina
dc.contributor.authorvan der Linden, Bart
dc.contributor.authorOuld-Chikh, Samy
dc.contributor.authorAguilar-Tapia, Antonio
dc.contributor.authorYarulina, Irina
dc.contributor.authorAbou-Hamad, Edy
dc.contributor.authorSneider, Yuri G.
dc.contributor.authorOlivos Suarez, Alma I.
dc.contributor.authorHazemann, Jean-Louis
dc.contributor.authorKapteijn, Freek
dc.contributor.authorGascon, Jorge
dc.date.accessioned2018-09-03T13:24:59Z
dc.date.available2018-09-03T13:24:59Z
dc.date.issued2018
dc.identifier.citationVollmer I, van der Linden B, Ould-Chikh S, Aguilar-Tapia A, Yarulina I, et al. (2018) On the dynamic nature of Mo sites for methane dehydroaromatization. Chemical Science 9: 4801–4807. Available: http://dx.doi.org/10.1039/c8sc01263f.
dc.identifier.issn2041-6520
dc.identifier.issn2041-6539
dc.identifier.doi10.1039/c8sc01263f
dc.identifier.urihttp://hdl.handle.net/10754/628454
dc.description.abstractThe mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active site formation was isolated from coke formation. With this a clear C NMR signal solely from the active site and not obscured by coke was obtained, and it revealed two types of likely molecular Mo (oxy-)carbidic species in addition to the β-MoC nanoparticles often mentioned in the literature. Furthermore, separating the active site formation from coking by pre-carburization helped us examine how methane is activated on the catalytic site by carrying out MDA using isotopically labelled methane (CH). Carbon originating from the pre-formed carbide was incorporated into the main products of the reaction, ethylene and benzene, demonstrating the dynamic behavior of the (oxy-)carbidic active sites.
dc.description.sponsorshipWe gratefully acknowledge the financial support from the Sabic- NWO CATC1CHEM CHIPP project. Thanks go to Dr Christoph Dittrich (SABIC), Dr Frank Mostert (SABIC) and Dr Xander Nijhuis (SABIC) as well as Prof. Emiel Hensen (TU Eindhoven) and Nikolay Kosinov (TU Eindhoven) for helpful discussion. We also acknowledge the BM26B DUBBLE beamline and the BM16 FAME-UHD beamline of the European Synchrotron Radiation Facility (ESRF), Grenoble, France for letting us use their facilities. Thanks also go to Maarten Gorseling (TU Delft) for performing GC-MS analysis. The FAME-UHD project is financially supported by the French "grand emprunt" EquipEx (EcoX, ANR- 10-EQPX-27-01), the CEA-CNRS CRG consortium and the INSU CNRS institute.
dc.publisherRoyal Society of Chemistry (RSC)
dc.relation.urlhttp://pubs.rsc.org/en/Content/ArticleLanding/2018/SC/C8SC01263F#!divAbstract
dc.rightsThis Open Access Article is licensed under a Creative Commons Attribution-Non Commercial 3.0 Unported Licence
dc.rights.urihttp://creativecommons.org/licenses/by-nc/3.0/
dc.titleOn the dynamic nature of Mo sites for methane dehydroaromatization
dc.typeArticle
dc.contributor.departmentChemical Engineering Program
dc.contributor.departmentCompetitive Research Funds
dc.contributor.departmentImaging and Characterization Core Lab
dc.contributor.departmentKAUST Catalysis Center (KCC)
dc.contributor.departmentNMR
dc.contributor.departmentOCRF- Special Academic Partnership
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalChemical Science
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionCatalysis Engineering, Chemical Engineering Department, Delft University of Technology, Van der Maasweg 9, Delft, 2629 HZ, , Netherlands
dc.contributor.institutionInst. Néel, UPR 2940 CNRS-Univ. Grenoble Alpes, Grenoble, F-38000, , , France
dc.contributor.institutionDipartimento di Ingegneria Chimica Materiali Ambiente, Sapienza Universitá di Roma, Via Eudossiana 18, Rome, 00184, , Italy
kaust.personOuld-Chikh, Samy
kaust.personYarulina, Irina
kaust.personAbou-Hamad, Edy
kaust.personGascon, Jorge
refterms.dateFOA2018-09-05T12:50:48Z


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