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Carbon quantum dots (CDs) are a relatively new class of carbon nanomaterials which have been studied very much in the last fifteen years to improve their already favorable properties. The optical properties of CDs have drawn particular interest as they display the unusual trait of excitation-dependent emission, as well as high fluorescence quantum yields (QY), long photoluminescence (PL) decay lifetimes, and photostability. These qualities naturally lead researchers to apply CDs in the field of imaging (particularly bio-imaging) and sensing. Since the amount of publications regarding CDs has been growing nearly exponentially in the last ten years, many improvements have been made in the optical properties of CDs such as QY and PL lifetime. However, a great deal of confusion remains regarding the PL mechanism of CDs as well as their structural properties. Therefore, presented in this review is a summary and discussion of the QYs and PL lifetimes reported in recent years. The effect of method as well as precursor has been evaluated and discussed appropriately. The current theories regarding the PL mechanism of CDs are discussed, with special attention to the concept of surface state-controlled PL. With this knowledge, the improvement of preparation and applications of CDs related to their optical properties will be easily accomplished. Further improvements can be made to CDs through the understanding of their structural and optical properties.
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A Review of Fluorescent Carbon Dots, Their Synthesis, Physical and Chemical Characteristics, and Applications
Carbon dots (CDs) are a particularly useful type of fluorescent nanoparticle that demonstrate biocompatibility, resistance to photobleaching, as well as diversity in composition and characteristics amongst the different types available. There are two main morphologies of CDs: Disk-shaped with 1–3 stacked sheets of aromatic carbon rings and quasi-spherical with a core-shell arrangement having crystalline and amorphous properties. They can be synthesized from various potentially environmentally friendly methods including hydrothermal carbonization, microwaving, pyrolysis or combustion, and are then purified via one or more methods. CDs can have either excitation wavelength-dependent or -independent emission with each having their own benefits in microscopic fluorescent imaging. Some CDs have an affinity for a particular cell type, organelle or chemical. This property allows the CDs to be used as sensors in a biological environment and can even provide quantitative information if the quenching or intensity of their fluorescence is dependent on the concentration of the analyte. In addition to fluorescent imaging, CDs can also be used for other applications including drug delivery, quality control, photodynamic therapy, and photocatalysis.
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- Award ID(s):
- 1849063
- PAR ID:
- 10285953
- Date Published:
- Journal Name:
- Nanomaterials
- Volume:
- 11
- Issue:
- 6
- ISSN:
- 2079-4991
- Page Range / eLocation ID:
- 1448
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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null (Ed.)Multicolor carbon dots (CDs) have been developed recently and demonstrate great potential in bio-imaging, sensing, and LEDs. However, the fluorescence mechanism of their tunable colors is still under debate, and efficient separation methods are still challenging. Herein, we synthesized multicolor polymeric CDs through solvothermal treatment of citric acid and urea in formamide. Automated reversed-phase column separation was used to achieve fractions with distinct colors, including blue, cyan, green, yellow, orange and red. This work explores the physicochemical properties and fluorescence origins of the red, green, and blue fractions in depth with combined experimental and computational methods. Three dominant fluorescence mechanism hypotheses were evaluated by comparing time-dependent density functional theory and molecular dynamics calculation results to measured characteristics. We find that blue fluorescence likely comes from embedded small molecules trapped in carbonaceous cages, while pyrene analogs are the most likely origin for emission at other wavelengths, especially in the red. Also important, upon interaction with live cells, different CD color fractions are trafficked to different sub-cellular locations. Super-resolution imaging shows that the blue CDs were found in a variety of organelles, such as mitochondria and lysosomes, while the red CDs were primarily localized in lysosomes. These findings significantly advance our understanding of the photoluminescence mechanism of multicolor CDs and help to guide future design and applications of these promising nanomaterials.more » « less
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Biomass-derived carbon dots (CDs) are biocompatible and have potential for a variety of applications, including bioimaging and biosensing. In this work, we use ground soybean residuals to synthesize carbon nanoparticles by hydrothermal carbonization (HTC), annealing at high temperature, and laser ablation (LA) in a NH 4 OH solution. The carbon nanoparticles synthesized with the HTC process (HTC-CDs) exhibit photoluminescent characteristics with strong blue emission. The annealing of the HTC-processed carbon particles in the range of 250 to 850 °C causes a loss of the photoluminescent characteristics of the CDs without any significant change in the microstructure (amorphous structure) of the carbon particles. The LA processing of the annealed HTC-processed carbon particles introduces nitrogen-containing surface-functional groups and leads to the recovery of the photoluminescent features that are different from those of the HTC-CDs and dependent on the fraction of nitrogen in the surface-functional groups. The photoluminescence of both the HTC-CDs and LA-CDs is largely due to the presence of N-containing surface-functional groups. The quantum yield of the LA-CDs is more constant than that of the HTC-CDs under continuous UV excitation and does not exhibit a significant reduction after 150 min of excitation. The methods used in this work provide a simple and green strategy to introduce N-surface-functional groups to carbon nanoparticles made from biomass and biowaste and to produce stable photoluminescent CDs with excellent water-wettability.more » « less
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The current preparation methods of carbon quantum dots (CDs) involve many reaction parameters, which leads to many possibilities in the synthesis processes and high uncertainty of the resultant production performance. Recently, machine learning (ML) methods have shown great potential in correlating the selected features in many applications, which can help understand the relevant structure–function relationships of CDs and discover better synthesis recipes as well. In this work, we employ the ML approach to guide the blue CD synthesis in microwave systems. After optimizing the synthesis parameters and conditions, the quantum yield (QY) increases to about 200% higher than the average value of the prepared samples without ML guidance. The obtained CDs are applied as fluorescent probes to monitor hydrogen peroxide (H 2 O 2 ) in human teeth. The CD probe exhibits a linear relationship with the concentration of H 2 O 2 ranging from 0 to 1.1 M with a lower detection limit of 0.12 M, which can effectively detect the residual H 2 O 2 after bleaching teeth. This work shows that the adopted ML methods have considerable advantages in guiding the synthesis of high-quality CDs, which could accelerate the development of other novel functional materials in energy, biomedical, and environmental remediation applications.more » « less
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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.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.3390/nano11061448
