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Designing Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates

TitoloDesigning Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates
Tipo di pubblicazioneArticolo su Rivista peer-reviewed
Anno di Pubblicazione2020
AutoriLimosani, F., Kaur R., Cataldo Antonino, Bellucci S., Micciulla F., Zanoni R., Lembo A., Wang B., Pizzoferrato R., Guldi D.M., and Tagliatesta P.
RivistaAngewandte Chemie - International Edition
Parole chiaveCharge 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

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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Citation KeyLimosani202023706