Electron-Transfer-Mediated Uranium Detection Using Quasi-Type II Core-Shell Quantum Dots: Insight into Mechanistic Pathways.

Uranium is one of the most toxic and important elements present in the environment, and because of its high toxicity, ultra-trace-level detection is of utmost importance. Many methods were reported earlier for this purpose, but each has its own limitations such as high cost, sophisticated instrumentation, sample processing, and so forth. Herein we have demonstrated an alternate method that is much simpler and can be used for the ultra-trace-level detection of uranium. We have synthesized 3-mercaptopropionic acid (MPA)-capped CdSe/CdS core-shell quantum dots (CSQDs) and used its photoluminescence properties to detect uranium in solution. Steady-state emission studies suggest the luminescence quenching of CSQDs in the presence of uranium. Redox levels of CSQDs and uranium suggests that the electron-transfer process from photoexcited CSQDs to uranium is a thermodynamically viable process, which has subsequently been confirmed by time-resolved studies. A Stern-Volmer plot of CSQDs with uranium suggests that the detection limit of this method is 74.5 ppb. The method has an advantage over other reported methods for being simple and low cost and requiring a small amout of sample processing. To the best of our knowledge, we are reporting for the first time uranium detection using quasi-type II CSQDs and proposing the mechanistic path through luminescence spectroscopy, which in turn helps us to design an efficient detection method.