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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. 

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. 

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. 

Carbon dots were originally found and reported as surface-passivated small carbon nanoparticles, where the effective surface passivation was the chemical functionalization of the carbon nanoparticles with organic molecules. Understandably, the very broad optical absorptions of carbon dots are largely the same as those intrinsic to the carbon nanoparticles, characterized by progressively decreasing absorptivities from shorter to longer wavelengths. Thus, carbon dots are generally weak absorbers in the red/near-IR and correspondingly weak emitters with low quantum yields. Much effort has been made on enhancing the optical performance of carbon dots in the red/near-IR, but without meaningful success due to the fact that optical absorptivities defined by Mother Nature are in general rather inert to any induced alterations. Nevertheless, there were shockingly casual claims in the literature on the major success in dramatically altering the optical absorption profiles of “carbon dots” by simply manipulating the dot synthesis to produce samples of some prominent optical absorption bands in the red/near-IR. Such claims have found warm receptions in the research field with a desperate need for carbon dots of the same optical performance in the red/near-IR as that in the green and blue. However, by looking closely at the initially reported synthesis and all its copies in subsequent investigations on the “red/near-IR carbon dots”, one would find that the “success” of the synthesis by thermal or hydrothermal carbonization processing requires specific precursor mixtures of citric acid with formamide or urea. In the study reported here, the systematic investigation included precursor mixtures of citric acid with not only formamide or urea but also their partially methylated or permethylated derivatives for the carbonization processing under conditions similar to and beyond those commonly used and reported in the literature. Collectively all of the results are consistent only with the conclusion that the origins of the observed red/near-IR optical absorptions in samples from some of the precursor mixtures must be molecular chromophores from thermally induced chemical reactions, nothing to do with any nanoscale carbon entities produced by carbonization. 

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. 

The antiviral function of carbon dots (CDots) with visible light exposure was evaluated, for which the model bacteriophages MS2 as a surrogate of small RNA viruses were used. The results show clearly that the visible light-activated CDots are highly effective in diminishing the infectivity of MS2 in both low and high titer samples to the host E. coli cells, and the antiviral effects are dot concentration- and treatment time-dependent. The action of CDots apparently causes no significant damage to the structural integrity and morphology of the MS2 phage or the breakdown of the capsid proteins, but does result in the protein carbonylation (a commonly used indicator for protein oxidation) and the degradation of viral genomic RNA. Mechanistically the results may be understood in the framework of photodynamic effects that are associated with the unique excited state properties and processes of CDots. Opportunities for potentially broad applications of CDots coupled with visible/natural light in the prevention and control of viral transmission and spread are highlighted and discussed.