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dc.contributor.authorPappas, Dimitrios
dc.contributor.authorBorfecchia, Elisa
dc.contributor.authorDyballa, Michael Martin
dc.contributor.authorPankin, Ilia A.
dc.contributor.authorLomachenko, Kirill A.
dc.contributor.authorMartini, Andrea
dc.contributor.authorSignorile, Matteo
dc.contributor.authorTeketel, Shewangizaw
dc.contributor.authorArstad, Bjørnar
dc.contributor.authorBerlier, Gloria
dc.contributor.authorLamberti, Carlo
dc.contributor.authorBordiga, Silvia
dc.contributor.authorOlsbye, Unni
dc.contributor.authorLillerud, Karl Petter
dc.contributor.authorSvelle, Stian
dc.contributor.authorBeato, Pablo
dc.date.accessioned2020-12-22T12:48:37Z
dc.date.available2020-12-22T12:48:37Z
dc.date.created2017-11-13T20:54:50Z
dc.date.issued2017
dc.identifier.citationJournal of the American Chemical Society. 2017, 139 (42), 14961-14975.en_US
dc.identifier.issn0002-7863
dc.identifier.urihttps://hdl.handle.net/11250/2720792
dc.description.abstractCu-exchanged zeolites possess active sites that are able to cleave the C–H bond of methane at temperatures ≤200 °C, enabling its selective partial oxidation to methanol. Herein we explore this process over Cu-SSZ-13 materials. We combine activity tests and X-ray absorption spectroscopy (XAS) to thoroughly investigate the influence of reaction parameters and material elemental composition on the productivity and Cu speciation during the key process steps. We find that the CuII moieties responsible for the conversion are formed in the presence of O2 and that high temperature together with prolonged activation time increases the population of such active sites. We evidence a linear correlation between the reducibility of the materials and their methanol productivity. By optimizing the process conditions and material composition, we are able to reach a methanol productivity as high as 0.2 mol CH3OH/mol Cu (125 μmol/g), the highest value reported to date for Cu-SSZ-13. Our results clearly demonstrate that high populations of 2Al Z2CuII sites in 6r, favored at low values of both Si:Al and Cu:Al ratios, inhibit the material performance by being inactive for the conversion. Z[CuIIOH] complexes, although shown to be inactive, are identified as the precursors to the methane-converting active sites. By critical examination of the reported catalytic and spectroscopic evidence, we propose different possible routes for active-site formation.en_US
dc.language.isoengen_US
dc.publisherAmerican Chemical Societyen_US
dc.subjectMaterialsen_US
dc.subjectExtractionen_US
dc.subjectAlcoholsen_US
dc.subjectHydrocarbonsen_US
dc.subjectX-ray absorption near edge spectroscopyen_US
dc.titleMethane to methanol: structure-activity relationships for Cu-CHAen_US
dc.typePeer revieweden_US
dc.typeJournal articleen_US
dc.description.versionacceptedVersionen_US
dc.rights.holderThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.7b06472en_US
dc.source.pagenumber14961-14975en_US
dc.source.volume139en_US
dc.source.journalJournal of the American Chemical Societyen_US
dc.source.issue42en_US
dc.identifier.doi10.1021/jacs.7b06472
dc.identifier.cristin1513677
dc.relation.projectNorges forskningsråd: 247730en_US
dc.relation.projectNorges forskningsråd: 237922en_US
cristin.unitcode7401,80,3,3
cristin.unitnameSorbentbaserte teknologier
cristin.ispublishedtrue
cristin.fulltextpostprint
cristin.qualitycode2


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