Counter-intuitive gas-phase reactivities of [V2]+ and [V2O]+ towards CO2 reduction: Insight from electronic structure calculations
| dc.contributor.author | Li, Jilai | |
| dc.contributor.author | Geng, Caiyun | |
| dc.contributor.author | Weiske, Thomas | |
| dc.contributor.author | Schwarz, Helmut | |
| dc.date.accessioned | 2021-06-03T14:17:25Z | |
| dc.date.available | 2021-06-03T14:17:25Z | |
| dc.date.issued | 2020-02-26 | |
| 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.sponsorship | DFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat" | en |
| dc.description.sponsorship | TU Berlin, Open-Access-Mittel – 2020 | en |
| dc.identifier.eissn | 1521-3757 | |
| dc.identifier.issn | 0044-8249 | |
| dc.identifier.uri | https://depositonce.tu-berlin.de/handle/11303/13197 | |
| dc.identifier.uri | http://dx.doi.org/10.14279/depositonce-11992 | |
| dc.language.iso | en | en |
| dc.rights.uri | https://creativecommons.org/licenses/by/4.0/ | en |
| dc.subject.ddc | 547 Organische Chemie | de |
| dc.subject.other | CO2 activation | en |
| dc.subject.other | gas-phase reactions | en |
| dc.subject.other | oxidation state | en |
| dc.subject.other | quantum chemical calculations | en |
| dc.title | Counter-intuitive gas-phase reactivities of [V2]+ and [V2O]+ towards CO2 reduction: Insight from electronic structure calculations | en |
| dc.type | Article | en |
| dc.type.version | publishedVersion | en |
| dcterms.bibliographicCitation.doi | 10.1002/anie.202001223 | en |
| dcterms.bibliographicCitation.issue | 30 | en |
| dcterms.bibliographicCitation.journaltitle | Angewandte Chemie | en |
| dcterms.bibliographicCitation.originalpublishername | Wiley | en |
| dcterms.bibliographicCitation.originalpublisherplace | New York, NY | en |
| dcterms.bibliographicCitation.pageend | 12314 | en |
| dcterms.bibliographicCitation.pagestart | 12308 | en |
| dcterms.bibliographicCitation.volume | 59 | en |
| tub.accessrights.dnb | free | en |
| tub.affiliation | Fak. 2 Mathematik und Naturwissenschaften::Inst. Chemie::FG Organische Chemie | de |
| tub.affiliation.faculty | Fak. 2 Mathematik und Naturwissenschaften | de |
| tub.affiliation.group | FG Organische Chemie | de |
| tub.affiliation.institute | Inst. Chemie | de |
| tub.publisher.universityorinstitution | Technische Universität Berlin | en |