Carbon quantum dots (CQDs) represent a class of carbon materials exhibiting photoresponse and many potential applications. Here, we present a unique property that dissolved CQDs capture large amounts of molecular oxygen from the air, the quantity of which can be controlled by light irradiation. The O content can be varied between a remarkable 1 wt % of the CQDs in the dark to nearly half of it under illumination, in a reversible manner. Moreover, O depletion enhances away from the air-solution interface as the nearby CQDs quickly regain them from the air, creating a pronounced concentration gradient in the solution. We elucidate the role of the CQD functional groups and show that excitons generated under light are responsible for their tunable adsorbed-oxygen content. Because of O enrichment, the photocatalytic efficiency of the CQDs toward oxidation of benzylamines in the air is the same as under oxygen flow and far higher than the existing photocatalysts. The findings should encourage the development of a new class of oxygen-enricher materials and air as a sustainable oxidant in chemical transformations.
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http://dx.doi.org/10.1021/jacs.1c10636 | DOI Listing |
Heliyon
January 2025
Transmission Electronic Microscopy Laboratory, Electronic Microscopy Unit, Department of Biology, University of Cauca, Popayán, 190002, Colombia.
A green methodology for the synthesis of carbon quantum dots (CQDs) from coffee husk without the use of any toxic solvents is proposed in this work. Sonochemical exfoliation of biochar, obtained from the thermal carbonization of coffee husk (from a certified coffee seeds) at low temperature in an air-restricted atmosphere, is described as an alternative procedure for the sustainable production of CQDs. The synthesized CQDs exhibited blue fluorescence with a strong maximum emission band at 410 nm when excited at a maximum absorption wavelength of 330 nm.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
University of Belgrade - Faculty of Chemistry, Studentski trg 12-16, Belgrade, Serbia.
Using high-level quantum chemical calculations, we predicted a strong O-H⋯C interaction between the apical carbon atoms of pyramidane and its derivatives and water molecules. Analysis of calculated electrostatic potential maps showed that there are areas of strong negative potential above apical carbon atoms in all studied structures. The results of quantum chemical calculations showed that the O-H⋯C interaction between the hydrogen atom of water and the apical carbon atom of pyramidane derivatives with four -CH substituents is unexpectedly strong, Δ = -7.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Instytut Chemii Organicznej PAN: Instytut Chemii Organicznej Polskiej Akademii Nauk, Institute of Organic Chemistry, Kasprzaka 44/52, 01-224, Warsaw, POLAND.
The development of straightforward synthetic methods for photoactive polycyclic aromatic hydrocarbons (PAHs) that avoid Pd-catalyzed or radical-based processes remains a challenge. Such methods are essential to reducing the cost and environmental impact of organic photodevices. In this work, we present a one-pot synthetic approach for creating novel bipolar PAHs with extended π-conjugation, which are not accessible via conventional Pd-catalyzed routes.
View Article and Find Full Text PDFJ Mater Chem B
January 2025
Center for Nano Science and Technology, Istituto Italiano di Tecnologia, 20134 Milano, Italy.
Carbon dots (CDs) are promising candidates as oxygen photosensitizers, in cancer therapeutic applications due to their high quantum yield, superior chemical and photostability, low cytotoxicity and ease of chemical functionalization/tuning. Nitrogen doping can further improve oxygen photosensitization performance. Besides photodynamic therapy, however, the possibility to finely and remotely regulate the intracellular redox balance by using physical stimuli has been attracting more and more interest not only for nanotheranostic application, but also as a novel, fully biocompatible therapeutic tool.
View Article and Find Full Text PDFNanoscale
January 2025
Chemistry Division, Bhabha Atomic Research Centre, Trombay, Mumbai-400085, India.
Sub-cellular organelle anomalies are frequently observed in diseases such as cancer. Early and precise diagnosis of these alterations can be crucial for patient outcomes. However, current diagnostic tools using conventional organic dyes or metal quantum dots face limitations, including poor biocompatibility, stringent storage conditions, limited solubility in aqueous media, and slow staining speeds.
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