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Nitrogen-Doped Carbon Nanodots Produced by Femtosecond Laser Synthesis for Effective Fluorophores.

ABSTRACT: Understanding the effect of heteroatom doping is crucial for the design of carbon nanodots (CNDs) with enhanced luminescent properties for fluorescence imaging and light-emitting devices. Here, we study the effect and mechanisms of luminescence enhancement through nitrogen doping in nanodots synthesized by the bottom-up route in an intense femtosecond laser field using the comparative analysis of CNDs obtained from benzene and pyridine. We demonstrate that laser irradiation of aromatic compounds produces hybrid nanoparticles consisting of a nanocrystalline core with a shell of surface-bonded aromatic rings. These nanoparticles exhibit excitation-dependent visible photoluminescence typical for CNDs. Incorporation of nitrogen into pyridine-derived CNDs enhances their luminescence characteristics through the formation of small pyridine-based fluorophores peripherally bonded to the nanoparticles. We identify oxidation of surface pyridine rings as a mechanism of formation of several distinct blue- and green-emitting fluorophores in nanodots, containing pyridine moieties. These findings shed additional light on the nature and formation mechanism of effective fluorophores in nitrogen-doped carbon nanodots produced by the bottom-up route.

SUBMITTER: Astafiev AA

PROVIDER: S-EPMC8892850 | biostudies-literature | 2022 Mar

REPOSITORIES: biostudies-literature

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Nitrogen-Doped Carbon Nanodots Produced by Femtosecond Laser Synthesis for Effective Fluorophores.

Astafiev Artyom A AA Shakhov Aleksander M AM Tskhovrebov Alexander G AG Shatov Alexander A Gulin Alexander A Shepel Denis D Nadtochenko Victor A VA

ACS omega 20220217 8

Understanding the effect of heteroatom doping is crucial for the design of carbon nanodots (CNDs) with enhanced luminescent properties for fluorescence imaging and light-emitting devices. Here, we study the effect and mechanisms of luminescence enhancement through nitrogen doping in nanodots synthesized by the bottom-up route in an intense femtosecond laser field using the comparative analysis of CNDs obtained from benzene and pyridine. We demonstrate that laser irradiation of aromatic compounds ...[more]

PMID: 35252675

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Project description:The current research mainly focuses on transforming low-quality waste into value-added nanomaterials and investigating various ways of utilising them. The hydrothermal preparation of highly fluorescent N-doped carbon dots (N-CDs) was obtained from the carboxymethylcellulose (CMC) of oil palm empty fruit bunches and linear-structured polyethyleneimines (LPEI). Transmission electron microscopy (TEM) analysis showed that the obtained N-CDs had an average size of 3.4 nm. The N-CDs were monodispersed in aqueous solution and were strongly fluorescent under the irradiation of ultra-violet light. A detailed description of the morphology and shape was established using Fourier transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS). It was shown that LPEI were successfully tuned the fluorescence (PL) properties of CDs in both the intrinsic and surface electronic structures, and enhanced the quantum yield (QY) up to 44%. The obtained N-CDs exhibited remarkable PL stability, long lifetime and pH-dependence behaviour, with the excitation/emission maxima of 350/465.5 nm. Impressively, PL enhancement and blue-shifted emission could be seen with the dilution of the original N-CDs solution. The obtained N-CDs were further applied as fluorescent probe for the identification of Cu2+ in aqueous media. The mechanism could be attributed to the particularly high thermodynamic affinity of Cu2+ for the N-chelate groups over the surface of N-CDs and the fast metal-to-ligand binding kinetics. The linear relationship between the relative quenching rate and the concentration of Cu2+ were applied between 1-30 µM, with a detection limit of 0.93 µM. The fluorescent probe was successfully applied for the detection of Cu2+ in real water. Moreover, a solid-state film of N-CDs was prepared in the presence of poly (vinyl alcohol) (PVA) polymer and found to be stable even after 72-h of continuous irradiation to UV-lamp. In contrast to the aqueous N-CDs, the composite film showed only an excitation independent property, with enhanced PL QY of around 47%. Due to the strong and stable emission nature of N-CDs in both aqueous and solid conditions, the obtained N-CDs are ideal for reducing the overall preparation costs and applying them for various biological and environmental applications in the future.

Dataset Information

Nitrogen-Doped Carbon Nanodots Produced by Femtosecond Laser Synthesis for Effective Fluorophores.

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Nitrogen-Doped Carbon Nanodots Produced by Femtosecond Laser Synthesis for Effective Fluorophores.

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