Cotransformation of Carbon Dots and Contaminant under Light in Aqueous Solutions: A Mechanistic Study

In this study, the photochemistry of carbon dots (CDs) and their effects on pollutant transformation were systematically examined. Diethyl phthalate (DEP) degradation was strongly enhanced by CDs under UV light, with the observed reaction rate constant (k(obs)) increased by 2.4-15.1-fold by CDs at a concentration of 0.5-10 mg/L. Electron paramagnetic resonance (EPR) spectrometry combined with free radical quenching experiments with various chemical probes indicated the production of reactive oxygen species (ROS), including hydroxyl radicals ((OH)-O-center dot), singlet oxygen (O-1(2)), and superoxide radical anions (O-2(center dot-)), and these contributed to the enhanced DEP degradation. Meanwhile, CDs were also degraded to low-molecular-weight species and partially mineralized to CO2 by ROS, as evidenced by Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) and total organic carbon (TOC) analysis, and transformation of CDs was accelerated by DEP. Furthermore, CDs were degraded rapidly under natural sunlight, accompanied by the formation of (OH)-O-center dot and O-1(2). Anions such as CO32-, NO3-, and Cl- had limited effects on transformation of CDs, while humic substances greatly inhibited this process. Our results indicate that photoreactions of CDs play an important role in influencing the transformation of pollutants and CDs themselves in the natural aquatic environment. The findings provide invaluable information for evaluating risks associated with the release of CDs into the natural environment.