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Design of Carbon Dots for Metal-free Photoredox Catalysis

  • Simone Cailotto
    Simone Cailotto
    Department of Molecular Sciences and Nanosystems, Università Ca’ Foscari Venezia, Via Torino 155, 30172 Venezia Mestre, Italy
  • Raffaello Mazzaro
    Raffaello Mazzaro
    Division of Materials Science, Department of Engineering Sciences and Mathematics, Luleå University of Technology, 971 87 Luleå, Sweden
  • Francesco Enrichi
    Francesco Enrichi
    Museo Storico della Fisica e Centro Studi e Ricerche “Enrico Fermi”, Piazza del Viminale 1, 00184 Roma, Italy
    Division of Materials Science, Department of Engineering Sciences and Mathematics, Luleå University of Technology, 971 87 Luleå, Sweden
  • Alberto Vomiero
    Alberto Vomiero
    Division of Materials Science, Department of Engineering Sciences and Mathematics, Luleå University of Technology, 971 87 Luleå, Sweden
  • Maurizio Selva
    Maurizio Selva
    Department of Molecular Sciences and Nanosystems, Università Ca’ Foscari Venezia, Via Torino 155, 30172 Venezia Mestre, Italy
  • Elti Cattaruzza
    Elti Cattaruzza
    Department of Molecular Sciences and Nanosystems, Università Ca’ Foscari Venezia, Via Torino 155, 30172 Venezia Mestre, Italy
  • Davide Cristofori
    Davide Cristofori
    Department of Molecular Sciences and Nanosystems, Università Ca’ Foscari Venezia, Via Torino 155, 30172 Venezia Mestre, Italy
    Centro di microscopia elettronica “G. Stevanato”, Via Torino 155b, 30172 Venezia-Mestre, Italy
  • Emanuele Amadio*
    Emanuele Amadio
    Department of Molecular Sciences and Nanosystems, Università Ca’ Foscari Venezia, Via Torino 155, 30172 Venezia Mestre, Italy
    *E-mail: [email protected] (E.A.).
  • , and 
  • Alvise Perosa*
    Alvise Perosa
    Department of Molecular Sciences and Nanosystems, Università Ca’ Foscari Venezia, Via Torino 155, 30172 Venezia Mestre, Italy
    *E-mail: [email protected]. Phone: (+39) 041 234 8958. Fax: (+39) 041 234 8979 (A.P.).
Cite this: ACS Appl. Mater. Interfaces 2018, 10, 47, 40560–40567
Publication Date (Web):October 29, 2018
Copyright © 2018 American Chemical Society

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    Abstract Image

    The photoreduction potential of a set of four different carbon dots (CDs) was investigated. The CDs were synthesized by using two different preparation methods—hydrothermal and pyrolytic—and two sets of reagents—neat citric acid and citric acid doped with diethylenetriamine. The hydrothermal syntheses yielded amorphous CDs, which were either nondoped (a-CDs) or nitrogen-doped (a-N-CDs), whereas the pyrolytic treatment afforded graphitic CDs, either non-doped (g-CDs) or nitrogen-doped (g-N-CDs). The morphology, structure, and optical properties of four different types of CDs revealed significant differences depending on the synthetic pathway. The photocatalytic activities of the CDs were investigated as such, that is, in the absence of any other redox mediators, on the model photoreduction reaction of methyl viologen. The observed photocatalytic reaction rates: a-N-CDsg-CDs > a-CDsg-N-CDs were correlated with the presence/absence of fluorophores, to the graphitic core, and to quenching interactions between the two. The results indicate that nitrogen doping reverses the photoredox reactivity between amorphous and graphitic CDs and that amorphous N-doped CDs are the most photoredox active, a yet unknown fact that demonstrates the tunable potential of CDs for ad hoc applications.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.8b14188.

    • Detailed CDs synthesis and procedure optimization, UV–vis, PL, FT-IR, and XPS spectra; 2D-DOSY NMR interpretations; steady-state and time-resolved PL; CD–MV quenching experiments; photocatalytic blank reaction; and study on the induction time, mass absorption coefficient, and ζ-potential (PDF)

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