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.

Limosani, F., Kaur, R., Cataldo, A., Bellucci, S., Micciulla, F., Zanoni, R., et al. (2020). Designing cascades of electron transfer processes in multicomponent graphene conjugates. ANGEWANDTE CHEMIE, 59(52), 23706-23715 [10.1002/anie.202008820].

Designing cascades of electron transfer processes in multicomponent graphene conjugates

Limosani F.;Pizzoferrato R.;Tagliatesta P.
2020

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.
Pubblicato
Rilevanza internazionale
Articolo
Esperti anonimi
Settore CHIM/03
English
graphene nanoplates
zinc-tetraphenylporphyrin
Limosani, F., Kaur, R., Cataldo, A., Bellucci, S., Micciulla, F., Zanoni, R., et al. (2020). Designing cascades of electron transfer processes in multicomponent graphene conjugates. ANGEWANDTE CHEMIE, 59(52), 23706-23715 [10.1002/anie.202008820].
Limosani, F; Kaur, R; Cataldo, A; Bellucci, S; Micciulla, F; Zanoni, R; Lembo, A; Wang, B; Pizzoferrato, R; Guldi, Dm; Tagliatesta, P
Articolo su rivista
File in questo prodotto:
File Dimensione Formato  
anie.202008820.pdf

accesso aperto

Tipologia: Versione Editoriale (PDF)
Licenza: Creative commons
Dimensione 2.76 MB
Formato Adobe PDF
2.76 MB Adobe PDF Visualizza/Apri

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2108/264755
Citazioni
  • ???jsp.display-item.citation.pmc??? 4
  • Scopus 8
  • ???jsp.display-item.citation.isi??? 6
social impact