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Red, Yellow, and Blue Luminescence by Graphene Quantum Dots: Syntheses, Mechanism, and Cellular Imaging

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† State Key Laboratory of Virology & Key Laboratory of Analytical Chemistry for Biology and Medicine, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, P. R. China
‡ School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China
§ College of Chemistry and Material Science, Guangxi Teachers Education University, Nanning 530001, P. R. China
*Email: [email protected]. Tel: +86-27-68756667 (F.L.J.).
*E-mail: [email protected]. Tel: +86-27-68753465 (Y.L.).
Cite this: ACS Appl. Mater. Interfaces 2017, 9, 29, 24846–24856
Publication Date (Web):July 5, 2017
https://doi.org/10.1021/acsami.7b05569
Copyright © 2017 American Chemical Society
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    Abstract

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    Owing to their excellent photoluminescence (PL) properties, good biocompatibility, and low toxicity, graphene quantum dots (GQDs) are widely applied in bioimaging, biosensing, and so forth. However, further development of GQDs is limited by their synthetic methodology and unclear PL mechanism. Therefore, it is urgent to find efficient and universal methods for the synthesis of GQDs with high stability, controllable surface properties, and tunable PL emission wavelength. By coating with polyethyleneimine (PEI) of different molecular weights, blue-, yellow-, and red-emitting GQDs were successfully prepared. By transmission electron microscopy, atomic force microscopy, and dynamic light scattering, the characterization of size and morphology revealed that blue-emitting PEI1800 GQDs were monocoated, like jelly beans, and red-emitting PEI600 GQDs were multicoated, like capsules. The amidation reaction between carboxyl and amide functional groups played an important role in the coating process, as evidenced by IR spectroscopy and theoretical calculation with density functional theory B3LYP/6-31G*. The PL-tunable GQDs exhibited an excellent chemical stability and extremely low cytotoxicity, and they had been shown to be feasible for bioimaging, making these GQDs highly attractive for a wide variety of applications, including multicolor imaging and bioanalysis.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.7b05569.

    • Syntheses process (Figure S1); photos of GQDs powder (Figure S2); excitation-dependent PL spectra and PL spectra under UV lamp (Figure S3); XPS and HRXPS (Figure S4), elemental content analyses (Table S1), XRD spectra (Figure S5), zeta potential (Figure S6) of GQDS; schematic diagram of the key reaction (Figure S7); theoretical calculation results (Figure S8), energy gap information (Table S2), PL lifetime and chemical and optical stability of GQDs (Figure S9); biological stability and the toxicity test of GQDs (Figure S10); QY measurements of GQDs (Figure S11 and Table S3) (PDF)

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