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dc.contributor.authorGutterød, Emil Sebastian
dc.contributor.authorLazzarini, Andrea
dc.contributor.authorFjermestad, Torstein
dc.contributor.authorKaur, Gurpreet
dc.contributor.authorManzoli, Maela
dc.contributor.authorBordiga, Silvia
dc.contributor.authorSvelle, Stian
dc.contributor.authorLillerud, Karl Petter
dc.contributor.authorSkúlason, Egill
dc.contributor.authorØien-Ødegaard, Sigurd
dc.contributor.authorNova, Ainara
dc.contributor.authorOlsbye, Unni
dc.date.accessioned2020-01-24T14:39:47Z
dc.date.available2020-01-24T14:39:47Z
dc.date.created2020-01-20T16:45:34Z
dc.date.issued2019
dc.identifier.citationJournal of the American Chemical Society. 2020, 142 999-?.nb_NO
dc.identifier.issn0002-7863
dc.identifier.urihttp://hdl.handle.net/11250/2637885
dc.description.abstractMetal–organic frameworks (MOFs) show great prospect as catalysts and catalyst support materials. Yet, studies that address their dynamic, kinetic, and mechanistic role in target reactions are scarce. In this study, an exceptionally stable MOF catalyst consisting of Pt nanoparticles (NPs) embedded in a Zr-based UiO-67 MOF was subject to steady-state and transient kinetic studies involving H/D and 13C/12C exchange, coupled with operando infrared spectroscopy and density functional theory (DFT) modeling, targeting methanol formation from CO2/H2 feeds at 170 °C and 1–8 bar pressure. The study revealed that methanol is formed at the interface between the Pt NPs and defect Zr nodes via formate species attached to the Zr nodes. Methanol formation is mechanistically separated from the formation of coproducts CO and methane, except for hydrogen activation on the Pt NPs. Careful analysis of transient data revealed that the number of intermediates was higher than the number of open Zr sites in the MOF lattice around each Pt NP. Hence, additional Zr sites must be available for formate formation. DFT modeling revealed that Pt NP growth is sufficiently energetically favored to enable displacement of linkers and creation of open Zr sites during pretreatment. However, linker displacement during formate formation is energetically disfavored, in line with the excellent catalyst stability observed experimentally. Overall, the study provides firm evidence that methanol is formed at the interface of Pt NPs and linker-deficient Zr6O8 nodes resting on the Pt NP surface.nb_NO
dc.language.isoengnb_NO
dc.publisherAmerican Chemical Societynb_NO
dc.subjectPlatinumnb_NO
dc.subjectAlcoholsnb_NO
dc.subjectMetal organic frameworksnb_NO
dc.subjectCatalystsnb_NO
dc.subjectHydrogenationnb_NO
dc.titleHydrogenation of CO2 to Methanol by Pt Nanoparticles Encapsulated in UiO-67: Deciphering the Role of the Metal−Organic Frameworknb_NO
dc.typeJournal articlenb_NO
dc.typePeer reviewednb_NO
dc.description.versionacceptedVersionnb_NO
dc.rights.holder“This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of the American Chemical Society, copyright © American Chemical Society after peer review. To access the final edited and published work see http://dx.doi.org/10.1021/jacs.9b10873nb_NO
dc.source.pagenumber999-1009nb_NO
dc.source.volume142nb_NO
dc.source.journalJournal of the American Chemical Societynb_NO
dc.source.issue2nb_NO
dc.identifier.doi10.1021/jacs.9b10873
dc.identifier.cristin1778336
dc.relation.projectNordforsk: 85378nb_NO
dc.relation.projectNorges forskningsråd: 250044nb_NO
dc.relation.projectNotur/NorStore: nn4654knb_NO
dc.relation.projectNorges forskningsråd: 262695nb_NO
dc.relation.projectNotur/NorStore: nn4683knb_NO
dc.relation.projectNorges forskningsråd: 250795nb_NO
cristin.unitcode7401,80,40,0
cristin.unitnameProsessteknologi
cristin.ispublishedtrue
cristin.fulltextpreprint
cristin.qualitycode2


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