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  1. Abstract

    Carbon dots are defined as small carbon nanoparticles with effective surface passivation via organic functionalization. The definition is literally a description of what carbon dots are originally found for the functionalized carbon nanoparticles displaying bright and colorful fluorescence emissions, mirroring those from similarly functionalized defects in carbon nanotubes. In literature more popular than classical carbon dots are the diverse variety of dot samples from “one‐pot” carbonization of organic precursors. On the two different kinds of samples from the different synthetic approaches, namely, the classical carbon dots versus those from the carbonization method, highlighted in this article are their shared properties and apparent divergences, including also explorations of the relevant sample structural and mechanistic origins for the shared properties and divergences. Echoing the growing evidence and concerns in the carbon dots research community on the major presence of organic molecular dyes/chromophores in carbonization produced dot samples, demonstrated and discussed in this article are some representative cases of dominating spectroscopic interferences due to the organic dye contamination that have led to unfound claims and erroneous conclusions. Mitigation strategies to address the contamination issues, including especially the use of more vigorous processing conditions in the carbonization synthesis, are proposed and justified.

     
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  2. Carbon dots (CDots) are small carbon nanoparticles with effective surface passivation by organic functionalization. In the reported work, the surface functionalization of preexisting small carbon nanoparticles with N-ethylcarbazole (NEC) was achieved by the NEC radical addition. Due to the major difference in microwave absorption between the carbon nanoparticles and organic species such as NEC, the nanoparticles could be selectively heated via microwave irradiation to enable the hydrogen abstraction in NEC to generate NEC radicals, followed by in situ additions of the radicals to the nanoparticles. The resulting NEC-CDots were characterized by microscopy and spectroscopy techniques including quantitative proton and 13C NMR methods. The optical spectroscopic properties of the dot sample were found to be largely the same as those of CDots from other organic functionalization schemes. The high structural stability of NEC-CDots benefiting from the radical addition functionalization is highlighted and discussed. 
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  3. Carbon dots (CDots) are generally defined as small-carbon nanoparticles with surface organic functionalization and their classical synthesis is literally the functionalization of preexisting carbon nanoparticles. Other than these “classically defined CDots”, however, the majority of the dot samples reported in the literature were prepared by thermal carbonization of organic precursors in mostly “one-pot” processing. In this work, thermal processing of the selected precursors intended for carbonization was performed with conditions of 200 °C for 3 h, 330 °C for 6 h, and heating by microwave irradiation, yielding samples denoted as CS200, CS330, and CSMT, respectively. These samples are structurally different from the classical CDots and should be considered as “nano-carbon/organic hybrids”. Their optical spectroscopic properties were found comparable to those of the classical CDots, but very different in the related photoinduced antibacterial activities. Mechanistic origins of the divergence were explored, with the results suggesting major factors associated with the structural and morphological characteristics of the hybrids. 
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  4. The carbon/TiO2 hybrid dots (C/TiO2-Dots) are structurally TiO2 nanoparticles (in the order of 25 nm in diameter from commercially available colloidal TiO2 samples) surface-attached by nanoscale carbon domains with organic moieties, thus equivalent to hybrids of individual TiO2 nanoparticles each decorated with many carbon dots. These hybrid dots with exposure to visible light exhibit potent antibacterial properties, similar to those found in neat carbon dots with the same light activation. The results from the use of established scavengers for reactive oxygen species (ROS) to “quench” the antibacterial activities, an indication for shared mechanistic origins, are also similar. The findings in experiments on probing biological consequences of the antibacterial action suggest that the visible light-activated C/TiO2-Dots cause significant damage to the bacterial cell membrane, resulting in higher permeability, with the associated oxidative stress leading to lipid peroxidation, inhibiting bacterial growth. The induced bacterial cell damage could be observed more directly in the transmission electron microscopy (TEM) imaging. Opportunities for the further development of the hybrid dots platform for a variety of antibacterial applications are discussed. 
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  5. Carbon “quantum” dots or carbon dots (CDots) exploit and enhance the intrinsic photoexcited state properties and processes of small carbon nanoparticles via effective nanoparticle surface passivation by chemical functionalization with organic species. The optical properties and photoinduced redox characteristics of CDots are competitive to those of established conventional semiconductor quantum dots and also fullerenes and other carbon nanomaterials. Highlighted here are major advances in the exploration of CDots for their serving as high-performance yet nontoxic fluorescence probes for one- and multi-photon bioimaging in vitro and in vivo, and for their uniquely potent antimicrobial function to inactivate effectively and efficiently some of the toughest bacterial pathogens and viruses under visible/natural or ambient light conditions. Opportunities and challenges in the further development of the CDots platform and related technologies are discussed. 
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  6. This study aimed to address the significant problems of bacterial biofilms found in medical fields and many industries. It explores the potential of classic photoactive carbon dots (CDots), with 2,2′-(ethylenedioxy)bis (ethylamine) (EDA) for dot surface functionalization (thus, EDA-CDots) for their inhibitory effect on B. subtilis biofilm formation and the inactivation of B. subtilis cells within established biofilm. The EDA-CDots were synthesized by chemical functionalization of selected small carbon nanoparticles with EDA molecules in amidation reactions. The inhibitory efficacy of CDots with visible light against biofilm formation was dependent significantly on the time point when CDots were added; the earlier the CDots were added, the better the inhibitory effect on the biofilm formation. The evaluation of antibacterial action of light-activated EDA-CDots against planktonic B. subtilis cells versus the cells in biofilm indicate that CDots are highly effective for inactivating planktonic cells but barely inactivate cells in established biofilms. However, when coupling with chelating agents (e.g., EDTA) to target the biofilm architecture by breaking or weakening the EPS protection, much enhanced photoinactivation of biofilm-associated cells by CDots was achieved. The study demonstrates the potential of CDots to prevent the initiation of biofilm formation and to inhibit biofilm growth at an early stage. Strategic combination treatment could enhance the effectiveness of photoinactivation by CDots to biofilm-associated cells. 
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  7. Björkroth, Johanna (Ed.)
    ABSTRACT Foodborne pathogens have long been recognized as major challenges for the food industry and repeatedly implicated in food product recalls and outbreaks of foodborne diseases. This study demonstrated the application of a recently discovered class of visible-light-activated carbon-based nanoparticles, namely, carbon dots (CDots), for photodynamic inactivation of foodborne pathogens. The results demonstrated that CDots were highly effective in the photoinactivation of Listeria monocytogenes in suspensions and on stainless steel surfaces. However, it was much less effective for Salmonella cells, but treatments with higher CDot concentrations and longer times were still able to inactivate Salmonella cells. The mechanistic implications of the observed different antibacterial effects on the two types of cells were assessed, and the associated generation of intracellular reactive oxygen species (ROS), the resulting lipid peroxidation, and the leakage of nucleic acid and proteins from the treated cells were analyzed, with the results collectively suggesting CDots as a class of promising photodynamic inactivation agents for foodborne pathogens. IMPORTANCE Foodborne infectious diseases have long been recognized as major challenges in public health. Contaminations of food processing facilities and equipment with foodborne pathogens occur often. There is a critical need for new tools/approaches to control the pathogens and prevent such contaminations in food processing facilities and other settings. This study reports a newly established antimicrobial nanomaterials platform, CDots coupled with visible/natural light, for effective and efficient inactivation of representative foodborne bacterial pathogens. The study will contribute to promoting the practical application of CDots as a new class of promising nanomaterial-based photodynamic inactivation agents for foodborne pathogens. 
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  8. null (Ed.)
    Carbon dots (CDots) are defined as surface-passivated small carbon nanoparticles, with the effective passivation generally achieved by organic functionalization. Photoexcited CDots are both potent electron donors and acceptors, and their characteristic bright and colorful fluorescence emissions make them excellent fluorescence sensors for organic analytes and metal ions. For the latter extraordinarily low detection limits based on extremely efficient quenching of fluorescence intensities by the targeted metal cations have been observed and reported in the literature. However, all of the dot samples in those reported studies were made from “one-pot” carbonization of organic precursors mostly under rather mild processing conditions, unlikely to be sufficient for the required level of carbonization. Those dot samples should therefore be more appropriately considered as “nano-carbon/organic hybrids”, characterized structurally as being highly porous and spongy, which must be playing a dominating role in the reported sensing results. In this study, we compared the dot samples from carbonization syntheses under similarly mild and also more aggressive processing conditions with the classically defined and structured CDots for the fluorescence sensing of copper( ii ) cations in aqueous solutions. The observed dramatic decoupling between quenching results for fluorescence intensities and lifetimes of the carbonization samples, with the former being extraordinary and the latter within the diffusion controlled limit, suggested that the quenching of fluorescence intensities was greatly affected by the higher local quencher concentrations than the bulk associated with the porous and spongy sample structures, especially for the sample from carbonization under too mild processing conditions. The major differences between the classical CDots and the nano-carbon/organic hybrids are highlighted, and the tradeoffs between sensitivity and accuracy or reproducibility in the use of the latter for fluorescence sensing are discussed. 
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