• 文献标题:   Designing Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates
  • 文献类型:   Article
  • 作  者:   LIMOSANI F, KAUR R, CATALDO A, BELLUCCI S, MICCIULLA F, ZANONI R, LEMBO A, WANG BZ, PIZZOFERRATO R, GULDI DM, TAGLIATESTA P
  • 作者关键词:   graphene nanoplate, zinctetraphenylporphyrin
  • 出版物名称:   ANGEWANDTE CHEMIEINTERNATIONAL EDITION
  • ISSN:   1433-7851 EI 1521-3773
  • 通讯作者地址:   Univ Roma Tor Vergata
  • 被引频次:   0
  • DOI:   10.1002/anie.202008820 EA OCT 2020
  • 出版年:   2020

▎ 摘  要

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 beta-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.