Counter-intuitive gas-phase reactivities of [V2]+ and [V2O]+ towards CO2 reduction: Insight from electronic structure calculations

dc.contributor.authorLi, Jilai
dc.contributor.authorGeng, Caiyun
dc.contributor.authorWeiske, Thomas
dc.contributor.authorSchwarz, Helmut
dc.date.accessioned2021-06-03T14:17:25Z
dc.date.available2021-06-03T14:17:25Z
dc.date.issued2020-02-26
dc.description.abstract[V2O]+ remains “invisible” in the thermal gas-phase reaction of bare [V2]+ with CO2 giving rise to [V2O2]+; this is because the [V2O]+ intermediate is being consumed more than 230 times faster than it is generated. However, the fleeting existence of [V2O]+ and its involvement in the [V2]+ → [V2O2]+ chemistry are demonstrated by a cross-over labeling experiment with a 1:1 mixture of C16O2/C18O2, generating the product ions [V216O2]+, [V216O18O]+, and [V218O2]+ in a 1:2:1 ratio. Density functional theory (DFT) calculations help to understand the remarkable and unexpected reactivity differences of [V2]+ versus [V2O]+ towards CO2.en
dc.description.sponsorshipDFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat"en
dc.description.sponsorshipTU Berlin, Open-Access-Mittel – 2020en
dc.identifier.eissn1521-3757
dc.identifier.issn0044-8249
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/13197
dc.identifier.urihttp://dx.doi.org/10.14279/depositonce-11992
dc.language.isoenen
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/en
dc.subject.ddc547 Organische Chemiede
dc.subject.otherCO2 activationen
dc.subject.othergas-phase reactionsen
dc.subject.otheroxidation stateen
dc.subject.otherquantum chemical calculationsen
dc.titleCounter-intuitive gas-phase reactivities of [V2]+ and [V2O]+ towards CO2 reduction: Insight from electronic structure calculationsen
dc.typeArticleen
dc.type.versionpublishedVersionen
dcterms.bibliographicCitation.doi10.1002/anie.202001223en
dcterms.bibliographicCitation.issue30en
dcterms.bibliographicCitation.journaltitleAngewandte Chemieen
dcterms.bibliographicCitation.originalpublishernameWileyen
dcterms.bibliographicCitation.originalpublisherplaceNew York, NYen
dcterms.bibliographicCitation.pageend12314en
dcterms.bibliographicCitation.pagestart12308en
dcterms.bibliographicCitation.volume59en
tub.accessrights.dnbfreeen
tub.affiliationFak. 2 Mathematik und Naturwissenschaften>Inst. Chemie>FG Organische Chemiede
tub.affiliation.facultyFak. 2 Mathematik und Naturwissenschaftende
tub.affiliation.groupFG Organische Chemiede
tub.affiliation.instituteInst. Chemiede
tub.publisher.universityorinstitutionTechnische Universität Berlinen
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