Carbon dots are an emerging class of nanomaterials that has recently attracted considerable attention for applications that span from biomedicine to energy. These photoluminescent carbon nanoparticles are defined by characteristic sizes of <10 nm, a carbon-based core and various functional groups at their surface. Although the surface groups are widely used to establish non-covalent bonds (through electrostatic interactions, coordinative bonds, and hydrogen bonds) with various other (bio)molecules and polymers, the carbonaceous core could also establish non-covalent bonds (ππ stacking or hydrophobic interactions) with π-extended or apolar compounds. The surface functional groups, in addition, can be modified by various post-synthetic chemical procedures to fine-tune the supramolecular interactions. Our contribution categorizes and analyzes the interactions that are commonly used to engineer carbon dots-based materials and discusses how they have allowed preparation of functional assemblies and architectures used for sensing, (bio)imaging, therapeutic applications, catalysis, and devices. Using non-covalent interactions as a bottom-up approach to prepare carbon dots-based assemblies and composites can exploit the unique features of supramolecular chemistry, which include adaptability, tunability, and stimuli-responsiveness due to the dynamic nature of the non-covalent interactions. It is expected that focusing on the various supramolecular possibilities will influence the future development of this class of nanomaterials.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/smll.202300906

Supramolecular Chemistry of Carbon-Based Dots Offers Widespread Opportunities.

A sustainable approach for heavy metal remediation from water using Carbon Dot based Composites: A Review

Photocatalysis is an emerging field that exploits light-absorbing catalysts to yield transformations not even achievable in the dark. Considering the drawbacks of metal-based photocatalysts, Carbon Dots (CDs) recently emerged as suitable green alternatives for different photocatalytic reactions. These carbon nanoparticles are easy to prepare, non-toxic and potentially recyclable. Moreover, CDs usually display core-shell structures which are highly tunable via synthetic and post-synthetic strategies. This Concept Article focuses on the recent advancements in the CD-based photocatalysis, highlighting the link between their superficial and core composition and their resulting photo-redox abilities, and giving future perspectives on their application in cutting-edge areas. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/cctc.202300667

Shining Light on Carbon Dots: New Opportunities in Photocatalysis

Preparation strategies, optical properties, and sensing application of multicolor carbon dots. 

Synthetic strategies, properties and sensing application of multicolor carbon dots: recent advances and future challenges.

Elucidating the mechanism of surface nitrogen and sulfur modulation in multicolor carbon dots via electrochemical methods for information encryption applications. 

Electrochemical synthesis of fluorescence-enhanced carbon dots with multicolor emission via surface nitrogen and sulfur modulation for information encryption applications

ConspectusFluorescence is the emission of light following photon absorption. This optical phenomenon has many applications in daily life, such as in LED lamps, forensics, and bioimaging. Traditionally, small-molecule fluorophores were most common, but the types of molecules and particles with compelling fluorescence properties have expanded. For example, green fluorescent protein (GFP) was isolated from jellyfish and won the Nobel prize in 2008 due to its significant utility as a fluorescent biomarker. Using the intrinsic fluorescence of GFP, many previously invisible biological processes and substances can now be observed and studied. Other fluorescent materials have also been developed, greatly expanding the potential applications. Semiconductor quantum dots (QDs), which have bright fluorescence and a narrow bandwidth, are a popular choice for display technologies. However, QDs are made of heavy metal elements such as Cd and Se, which pose potential safety concerns to the environment and human health. Thus, new fluorescent organic materials are being developed to mitigate the toxicological concerns while maintaining the QD advantages.One type of new material attracting great attention as an environmentally friendly substitute for semiconductor QDs is carbon dots (CDs). CDs have been developed with strong fluorescence, good photostability, and low toxicity using a variety of precursors, and some synthesis processes have good potential for scale-up. However, since they are made of a variety of materials and through different methods, the structure and properties of CDs can differ from preparation to preparation. There are three major types of CDs: graphene quantum dots (GQDs), carbon quantum dots (CQDs), and amorphous or polymeric carbon dots (PCDs). This Account focuses on PCDs and their unique properties by comparing it with other types of CDs. The synthesis processes, fluorescence properties, fluorescence mechanisms, and toxicity are discussed below with an emphasis on the distinct attributes of PCDs.PCDs can be synthesized from small molecules or polymers. They have an amorphous or cross-linked polymer structure with bright fluorescence. This fluorescence is possibly due to cross-link-enhanced emission or clusteroluminescence that arises from the through-space interactions of heteroatomic-rich functional groups. Other fluorescence mechanisms of CDs, including distinct contributions from the carbon core and surface states, may also contribute. The toxicological profiles of CDs are influenced by the chemical composition, surface functionalization, and light illumination. CDs are generally thought to be of low toxicity, and this can be further improved by removing toxic byproducts, functionalizing the surface, and reducing light exposure to minimize the generation of reactive oxygen species.

Synthesis Processes, Photoluminescence Mechanism, and the Toxicity of Amorphous or Polymeric Carbon Dots.

Reactive oxygen species (ROS) are a set of oxygen- and nitrogen-containing radicals. They are produced from a wide range of sources. In biological contexts, cellular stress leads to an overproduction of ROS, which can lead to genetic damage and disease development. In industry, ROS are often productively used for water purification or for analyzing the possible toxicity of an industrial process. Because of their ubiquity, detection of ROS has been an analytical goal across a range of fields. To understand complicated systems and origins of ROS production, it is necessary to move from qualitative detection to quantitation. Analytical techniques that combine quantitation, high spatial and temporal resolution, and good specificity represent detection methods that can fill critical gaps in ROS research. Herein, we discuss the continued progress and limitations of fluorescence, electrochemical, and electron paramagnetic resonance detection of ROS over the last ten years, giving suggestions for the future of the field.

Progress and limitations in reactive oxygen species quantitation.

There is much concern about per- and polyfluoroalkyl substances (PFAS) based on their environmental persistence and toxicity, resulting in an urgent need for remediation technologies. This study focused on determining if nanoscale polymeric carbon dots are a viable sorbent material for PFAS and developing fluorine nuclear magnetic resonance spectroscopy (19F NMR) methods to probe interactions between carbon dots and PFAS at the molecular scale. Positively charged carbon dots (PEI-CDs) were synthesized using branched polyethyleneimine to target anionic PFAS by promoting electrostatic interactions. PEI-CDs were exposed to perfluorooctanoic acid (PFOA) to assess their potential as a PFAS sorbent material. After exposure to PFOA, the average size of the PEI-CDs increased (1.6 ± 0.5 to 7.8 ± 1.8 nm) and the surface charge decreased (+38.6 ± 1.1 to +26.4 ± 0.8 mV), both of which are consistent with contaminant sorption. 19F NMR methods were developed to gain further insight into PEI-CD affinity toward PFAS without any complex sample preparation. Changes in PFOA peak intensity and chemical shift were monitored at various PEI-CD concentrations to establish binding curves and determine the chemical exchange regime. 19F NMR spectral analysis indicates slow-intermediate chemical exchange between PFOA and CDs, demonstrating a high-affinity interaction. The α-fluorine had the greatest change in chemical shift and highest affinity, suggesting electrostatic interactions are the dominant sorption mechanism. PEI-CDs demonstrated affinity for a wide range of analytes when exposed to a mixture of 24-PFAS, with a slight preference toward perfluoroalkyl sulfonates. Overall, this study shows that PEI-CDs are an effective PFAS sorbent material and establishes 19F NMR as a suitable method to screen for novel sorbent materials and elucidate interaction mechanisms.

Using 19F NMR to Investigate Cationic Carbon Dot Association with Per- and Polyfluoroalkyl Substances (PFAS)


 Barium titanate (BTO) nanoparticles show great potential for use in electrostatic capacitors with high energy density. This includes both polymer composite and sintered capacitors. However, questions about the nanoparticles' size distribution, amount of agglomeration, and surface ligand effect on performance properties remain. Reducing particle agglomeration is a crucial step to understanding the properties of nanoscale particles, as agglomeration has significant effects on the composite dielectric constant. BTO surface functionalization using phosphonic acids is known reduce BTO nanoparticles agglomeration. We explore solution synthesized 10 nm BTO particles with tert-butylphosphonic acid ligands. Recent methods to quantifying agglomeration using an epoxy matrix before imaging shows that tert-butylphosphonic acid ligands reduce BTO agglomeration by 33%. Thermometric, spectroscopic, and computational methods provide confirmation of ligand binding and provide evidence of multiple ligand binding modes on the BTO particle surface.

Surface Functionalized Barium Titanate Nanoparticles: A Combined Experimental and Computational Study

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Papers

Synthesis Processes, Photoluminescence Mechanism, and the Toxicity of Amorphous or Polymeric Carbon Dots.

Progress and limitations in reactive oxygen species quantitation.

Using 19F NMR to Investigate Cationic Carbon Dot Association with Per- and Polyfluoroalkyl Substances (PFAS)

Surface Functionalized Barium Titanate Nanoparticles: A Combined Experimental and Computational Study