Designing Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates.

graphene nanoplates zinc-tetraphenylporphyrin

Journal

Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543

Informations de publication

Date de publication:
21 Dec 2020
Historique:
received: 24 06 2020
pubmed: 5 9 2020
medline: 5 9 2020
entrez: 5 9 2020
Statut: ppublish

Résumé

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.

Identifiants

pubmed: 32886436
doi: 10.1002/anie.202008820
pmc: PMC7756474
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

23706-23715

Subventions

Organisme : Deutsche Forschungsgemeinschaft
ID : SFB 953

Informations de copyright

© 2020 The Authors. Published by Wiley-VCH GmbH.

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Auteurs

Francesca Limosani (F)

Fusion and Nuclear Department, Photonics Micro and Nanostructures Laboratory, ENEA, Via E. Fermi 45, 00044 Frascati, Rome, Italy.
Department of Chemical Science and Technologies, University of Rome Tor Vergata, Via della Ricerca Scientifica 1, 00133, Rome, Italy.

Ramandeep Kaur (R)

Interdisciplinary Center for Molecular Materials, Department of Chemistry and Pharmacy, Friedrich-Alexander University Erlangen-Nürnberg, Egerlandstrasse 3, 91058, Erlangen, Germany.

Antonino Cataldo (A)

Department of Information Engineering, Polytechnic University of Marche, Via Brecce Bianche, 1, 60131, Ancona, Italy.
INFN- National laboratories of Frascati, Via Enrico Fermi 40, 00044 Frascati, Rome, Italy.

Stefano Bellucci (S)

INFN- National laboratories of Frascati, Via Enrico Fermi 40, 00044 Frascati, Rome, Italy.

Federico Micciulla (F)

Qi technologies, Via Monte D'Oro, 2/a, 00040, Pomezia, Italy.

Robertino Zanoni (R)

Department of Chemistry, University of Rome "La Sapienza", Piazzale Aldo Moro 5, 00185, Rome, Italy.

Angelo Lembo (A)

Department of Drug Metabolism and PharmacoKinetic, IRBM SpA, Via Pontina km 30.600, 00071 Pomezia, Rome, Italy.

Bingzhe Wang (B)

Interdisciplinary Center for Molecular Materials, Department of Chemistry and Pharmacy, Friedrich-Alexander University Erlangen-Nürnberg, Egerlandstrasse 3, 91058, Erlangen, Germany.

Roberto Pizzoferrato (R)

Department of Industrial Engineering, University of Rome Tor Vergata, Via del Politecnico 1, 00133, Rome, Italy.

Dirk M Guldi (DM)

Interdisciplinary Center for Molecular Materials, Department of Chemistry and Pharmacy, Friedrich-Alexander University Erlangen-Nürnberg, Egerlandstrasse 3, 91058, Erlangen, Germany.

Pietro Tagliatesta (P)

Department of Chemical Science and Technologies, University of Rome Tor Vergata, Via della Ricerca Scientifica 1, 00133, Rome, Italy.

Classifications MeSH