Abstract
Carbon dots (C-dots) are nanocarbon materials that exhibit a range of fluorescence and chemical/physical properties depending on the precursors employed and the conditions under which they were synthesized. However, the structural factors responsible for C-dot fluorescence remain unknown. This is because C-dots exhibit a wide distribution of sizes, structures, functional groups, heteroatoms, and defects, making structural analysis challenging. Therefore, a different experimental approach is necessary to explore the factors affecting the fluorescence. As a physicochemical approach, the surface properties of C-dots were altered by surface modification using organosilane, and the differences in fluorescence wavelength caused by the functionalization of C-dots were investigated in an organosilica matrix in this study. To explore the impact of varying chemical states of the C-dots surface on the fluorescence properties, it is necessary to evaluate them in a stable solid-state matrix that eliminates the effects of changes in the surrounding chemical state, dispersion state, and mobility. To compare the fluorescence properties, homogeneous hybrid organosilica films containing surface-functionalized C-dots were prepared using sol-gel method. For comparison, three types of C-dots were synthesized, each with a different fraction of surface reaction sites for functionalization. The fluorescence peak shift from pristine C-dots to functionalized C-dots in films was investigated for each. The reasons behind the fluorescence peak shifts and the local structures responsible for the fluorescence of the C-dots were explored based on the peak shift behavior and differences in the structural features of the as-prepared pristine C-dots.
Highlights
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Contribution of C-dot surface and core structures to fluorescence was experimentally investigated.
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Several C-dots with different surface states and similar fluorescence were synthesized.
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C-dots were functionalized with organoalkoxysilane changing their surface structures.
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The surface and core states of C-dots contribute to different fluorescence.
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Fluorescence peak shift behavior indicates common local structures for the different C-dots.
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Acknowledgements
The authors would like to thank Dr. S. Tanimoto (The University of Shiga Prefecture) for the technical support for DLS measurement.
Funding
This study was supported by JSPS bilateral joint research projects “MEAE-MESRI/SAKURA program” Grant Number JPJSBP120193218.
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Suzuki, K., Nabata, H., Ueno, S. et al. Origin of carbon dot fluorescence in organosilica films explored experimentally by surface functionalization. J Sol-Gel Sci Technol 104, 702–710 (2022). https://doi.org/10.1007/s10971-022-05901-1
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DOI: https://doi.org/10.1007/s10971-022-05901-1