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Designing Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates

TitleDesigning Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates
Publication TypeArticolo su Rivista peer-reviewed
Year of Publication2020
AuthorsLimosani, F., Kaur R., Cataldo Antonino, Bellucci S., Micciulla F., Zanoni R., Lembo A., Wang B., Pizzoferrato R., Guldi D.M., and Tagliatesta P.
JournalAngewandte Chemie - International Edition
Volume59
Pagination23706-23715
ISSN14337851
KeywordsCharge recombinations, Charge transfer, Charge-separated state, Delocalized electron, Electron transfer process, Electrons, Graphene, Organic polymers, Phenylene-ethynylenes, Physico-chemical characterization, Porphyrins, Redox reactions, Steady-state absorption, Transient absorption measurements
Abstract

A novel family of nanocarbon-based materials was designed, synthesized, and probed within the context of charge-transfer cascades. We integrated electron-donating ferrocenes with light-harvesting/electron-donating (metallo)porphyrins and electron-accepting graphene nanoplates (GNP) into multicomponent conjugates. To control the rate of charge flow between the individual building blocks, we bridged them via oligo-p-phenyleneethynylenes of variable lengths by β-linkages and the Prato–Maggini reaction. With steady-state absorption, fluorescence, Raman, and XPS measurements we realized the basic physico-chemical characterization of the photo- and redox-active components and the multicomponent conjugates. Going beyond this, we performed transient absorption measurements and corroborated by single wavelength and target analyses that the selective (metallo)porphyrin photoexcitation triggers a cascade of charge transfer events, that is, charge separation, charge shift, and charge recombination, to enable the directed charge flow. The net result is a few nanosecond-lived charge-separated state featuring a GNP-delocalized electron and a one-electron oxidized ferrocenium. © 2020 The Authors. Published by Wiley-VCH GmbH

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URLhttps://www.scopus.com/inward/record.uri?eid=2-s2.0-85092451569&doi=10.1002%2fanie.202008820&partnerID=40&md5=f23091926ab98e024c37a4859be1fab6
DOI10.1002/anie.202008820
Citation KeyLimosani202023706