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Article: Electron transfer and multi-electron accumulation in ExBox4+

TitleElectron transfer and multi-electron accumulation in ExBox<sup>4+</sup>
Authors
Keywordscyclophanes
electron transfer
ExBox
femtochemistry
photochemistry
Issue Date2014
Citation
Angewandte Chemie - International Edition, 2014, v. 53, n. 21, p. 5371-5375 How to Cite?
AbstractMolecules capable of accepting and storing multiple electrons are crucial components of artificial photosynthetic systems designed to drive catalysts, such as those used to reduce protons to hydrogen. ExBox4+, a boxlike cyclophane comprising two π-electron-poor extended viologen units tethered at both ends by two p-xylylene linkers, has been shown previously to accept an electron through space from a photoexcited guest. Herein is an investigation of an alternate, through-bond intramolecular electron-transfer pathway involving ExBox4+ using a combination of transient absorption and femtosecond stimulated Raman spectroscopy (FSRS). Upon photoexcitation of ExBox 4+, an electron is transferred from one of the p-xylylene linkers to one of the extended viologen units in ca. 240 ps and recombines in ca. 4 ns. A crystal structure of the doubly reduced species ExBox2+ was obtained. From outside the box: A viologen-based cyclophane ExBox4+ is photoexcited revealing a new through-bond pathway for electron transfer to ExBox4+. The solid-state structure with both redox states ExBox 4+ and ExBox2+ present, confirms that transferred electrons cause ExBox2+ to become flattened and form semiquinoidal structures capable of stabilizing unpaired electrons. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Persistent Identifierhttp://hdl.handle.net/10722/333075
ISSN
2023 Impact Factor: 16.1
2023 SCImago Journal Rankings: 5.300
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorDyar, Scott M.-
dc.contributor.authorBarnes, Jonathan C.-
dc.contributor.authorJuríček, Michal-
dc.contributor.authorStoddart, J. Fraser-
dc.contributor.authorCo, Dick T.-
dc.contributor.authorYoung, Ryan M.-
dc.contributor.authorWasielewski, Michael R.-
dc.date.accessioned2023-10-06T05:16:33Z-
dc.date.available2023-10-06T05:16:33Z-
dc.date.issued2014-
dc.identifier.citationAngewandte Chemie - International Edition, 2014, v. 53, n. 21, p. 5371-5375-
dc.identifier.issn1433-7851-
dc.identifier.urihttp://hdl.handle.net/10722/333075-
dc.description.abstractMolecules capable of accepting and storing multiple electrons are crucial components of artificial photosynthetic systems designed to drive catalysts, such as those used to reduce protons to hydrogen. ExBox4+, a boxlike cyclophane comprising two π-electron-poor extended viologen units tethered at both ends by two p-xylylene linkers, has been shown previously to accept an electron through space from a photoexcited guest. Herein is an investigation of an alternate, through-bond intramolecular electron-transfer pathway involving ExBox4+ using a combination of transient absorption and femtosecond stimulated Raman spectroscopy (FSRS). Upon photoexcitation of ExBox 4+, an electron is transferred from one of the p-xylylene linkers to one of the extended viologen units in ca. 240 ps and recombines in ca. 4 ns. A crystal structure of the doubly reduced species ExBox2+ was obtained. From outside the box: A viologen-based cyclophane ExBox4+ is photoexcited revealing a new through-bond pathway for electron transfer to ExBox4+. The solid-state structure with both redox states ExBox 4+ and ExBox2+ present, confirms that transferred electrons cause ExBox2+ to become flattened and form semiquinoidal structures capable of stabilizing unpaired electrons. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.-
dc.languageeng-
dc.relation.ispartofAngewandte Chemie - International Edition-
dc.subjectcyclophanes-
dc.subjectelectron transfer-
dc.subjectExBox-
dc.subjectfemtochemistry-
dc.subjectphotochemistry-
dc.titleElectron transfer and multi-electron accumulation in ExBox<sup>4+</sup>-
dc.typeArticle-
dc.description.naturelink_to_subscribed_fulltext-
dc.identifier.doi10.1002/anie.201402444-
dc.identifier.scopuseid_2-s2.0-84900794537-
dc.identifier.volume53-
dc.identifier.issue21-
dc.identifier.spage5371-
dc.identifier.epage5375-
dc.identifier.eissn1521-3773-
dc.identifier.isiWOS:000335809200021-

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