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 show selective luminescence. By contrast, acetic acid-derivedFluorescent 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.…
Verfasserangaben: | Till Thomas MeilingORCiDGND, Robin Mathis SchürmannORCiDGND, Stefanie VogelORCiDGND, Kenny EbelORCiD, Christophe Nicolas, Aleksandar R. Milosavljevic, Ilko BaldORCiDGND |
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DOI: | https://doi.org/10.1021/acs.jpcc.8b00748 |
ISSN: | 1932-7447 |
Titel des übergeordneten Werks (Englisch): | The journal of physical chemistry : C, Nanomaterials and interfaces |
Verlag: | American Chemical Society |
Verlagsort: | Washington |
Publikationstyp: | Wissenschaftlicher Artikel |
Sprache: | Englisch |
Datum der Erstveröffentlichung: | 10.05.2018 |
Erscheinungsjahr: | 2018 |
Datum der Freischaltung: | 01.12.2021 |
Band: | 122 |
Ausgabe: | 18 |
Seitenanzahl: | 14 |
Erste Seite: | 10217 |
Letzte Seite: | 10230 |
Fördernde Institution: | University of Potsdam; Deutsche Forschungsgemeinschaft (DFG)German Research Foundation (DFG); Synchrotron SOLEIL [20161220]; DFGGerman Research Foundation (DFG) [GSC 1013] |
Organisationseinheiten: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC-Klassifikation: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften |
Peer Review: | Referiert |