Carbon dots (CDs) are emerging as the material of choice in a range of applications due to their excellent photoluminescence properties, ease of preparation from inexpensive precursors, and low toxicity. However, the precise nature of the mechanism for the fluorescence is still under debate, and several molecular fluorophores have been reported. In this work, a new blue fluorophore, 5-oxopyrrolidine-3-carboxylic acid, was discovered in carbon dots synthesized from the most commonly used precursors: citric acid and urea. The molecular product alone has demonstrated interesting aggregation-enhanced emission (AEE), making it unique compared to other fluorophores known to be generated in CDs. We propose that this molecular fluorophore is associated with a polymer backbone within the CDs, and its fluorescence behavior is largely dependent on intermolecular interactions with the polymers or other fluorophores. Thus, a new class of non-traditional fluorophores is now relevant to the consideration of the CD fluorescence mechanism, providing both an additional challenge to the community in resolving the mechanism and an opportunity for a greater range of CD design schemes and applications.
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Identifying molecular fluorophore impurities in the synthesis of low-oxygen-content, carbon nanodots derived from pyrene
Carbon dots (C-dots) are a promising class of carbonaceous nanomaterials for bioimaging, catalysis, and optoelectronics. However, their applications are disrupted by recent reports that bright molecular fluorophores are co-produced in the synthesis of C-dots, in particular ones prepared through a bottom-up approach (carbon nanodots (CNDs)), commonly derived from citric acid precursors. The presence of highly emissive molecular fluorophore species obscures the true performance of CNDs and severely challenges the development of CNDs. Here we observe that the issue of molecular fluorophore impurity is still problematic for CNDs which are derived from a different type of precursor, polycylic aromatic hydrocarbons (PAHs). In this study, low-oxygen-content CNDs and small molecular fluorophores are co-produced through hydrothermal condensation of nitropyrene. Extensive and systematic characterization following column chromatographic separation and solvent-induced extraction reveals that molecular fluorophores and CNDs are clearly dissimilar in structure and optical properties. This work highlights that rigorous separation and purification steps need to be taken not only for hydrophilic CNDs but also for low-oxygen-content CNDs.
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- Award ID(s):
- 1854554
- PAR ID:
- 10430090
- Date Published:
- Journal Name:
- New Journal of Chemistry
- Volume:
- 46
- Issue:
- 17
- ISSN:
- 1144-0546
- Page Range / eLocation ID:
- 8324 to 8333
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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