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Photophysics and chemistry of nitrogen-doped carbon nanodots with high photoluminescence quantum yield

  • Fluorescent carbon nanodots (CNDs) are very promising nanomaterials for a broad range of applications because of their high photostability, presumed selective luminescence, and low cost at which they can be produced. In this respect, CNDs are superior to well-established semiconductor quantum dots and organic dyes. However, reported synthesis protocols for CNDs typically lead to low photoluminescence quantum yield (PLQY) and low reproducibility, resulting in a poor understanding of the CND chemistry and photophysics. Here, we report a one-step synthesis of nitrogen-doped carbon nanodots (N-CNDs) from various carboxylic acids, Tris, and ethylenediaminetetraacetic acid resulting in high PLQY of up to 90%. The reaction conditions in terms of starting materials, temperature, and reaction time are carefully optimized and their influence on the photophysical properties is characterized. We find that citric acid-derived N-CNDs can result in a very high PLQY of 90%, but they do not ShowFluorescent carbon nanodots (CNDs) are very promising nanomaterials for a broad range of applications because of their high photostability, presumed selective luminescence, and low cost at which they can be produced. In this respect, CNDs are superior to well-established semiconductor quantum dots and organic dyes. However, reported synthesis protocols for CNDs typically lead to low photoluminescence quantum yield (PLQY) and low reproducibility, resulting in a poor understanding of the CND chemistry and photophysics. Here, we report a one-step synthesis of nitrogen-doped carbon nanodots (N-CNDs) from various carboxylic acids, Tris, and ethylenediaminetetraacetic acid resulting in high PLQY of up to 90%. The reaction conditions in terms of starting materials, temperature, and reaction time are carefully optimized and their influence on the photophysical properties is characterized. We find that citric acid-derived N-CNDs can result in a very high PLQY of 90%, but they do not Show selective luminescence. By contrast, acetic acid-derived N-CNDs show selective luminescence but a PLQY of 50%. The chemical composition of the surface and core of these two selected N-CND types is characterized among others by high-Resolution synchrotron X-ray photoelectron spectroscopy using single isolated N-CND clusters. The results indicate that photoexcitation occurs in the N-CND core, whereas the emission properties are determined by the N-CND surface groups.zeige mehrzeige weniger

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Metadaten
Autor*innen:T. T. Meiling, Robin Schürmann, Stefanie Vogel, Kenny Ebel, C. Nicolas, A. R. Milosavljević, Ilko Bald
Dokumenttyp:Zeitschriftenartikel
Veröffentlichungsform:Verlagsliteratur
Sprache:Englisch
Titel des übergeordneten Werkes (Englisch):The Journal of Physical Chemistry C
Jahr der Erstveröffentlichung:2018
Organisationseinheit der BAM:1 Analytische Chemie; Referenzmaterialien
1 Analytische Chemie; Referenzmaterialien / 1.0 Abteilungsleitung und andere
Verlag:American Chemical Society
Verlagsort:Washington, DC
Jahrgang/Band:122
Ausgabe/Heft:18
Erste Seite:10217
Letzte Seite:10230
DDC-Klassifikation:Naturwissenschaften und Mathematik / Chemie / Analytische Chemie
Freie Schlagwörter:Carbon nanodots; Fluorescence; Synchrotron XPS
Themenfelder/Aktivitätsfelder der BAM:Chemie und Prozesstechnik
DOI:10.1021/acs.jpcc.8b00748
ISSN:1932-7447
Verfügbarkeit des Dokuments:Datei im Netzwerk der BAM verfügbar ("Closed Access")
Datum der Freischaltung:10.07.2018
Referierte Publikation:Ja
Datum der Eintragung als referierte Publikation:10.07.2018
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