Protein-directed synthesis of fluorescent sulfur quantum dots for highly robust detection of pyrophosphate

Inorganic pyrophosphate anions (PPi) play a key role in various biological processes and act as an essential indicator for physiological function evaluation and disease diagnosis. However, there is still a lack of available approaches for straightforward, robust, and convenient PPi detection. Herein, we design an on-off-on fluorescent switching nanoprobe employing Fe³⁺-mediated fluorescent sulfur quantum dots (SQDs) for highly robust detection of PPi. The bovine serum protein (BSA)-capped SQDs with fine water dispersibility and good optical stability are synthesized by an H₂O₂-assisted chemical etching reaction. Specifically, Fe³⁺ can strongly induce the aggregation of the SQDs into relatively larger sizes, resulting in aggregation-induced fluorescence quenching behavior. PPi can selectively bind with Fe³⁺ via emulative coordination and in preventing the aggregation of SQDs this is accompanied by recovery of fluorescence. The physicochemical properties of aggregated and disaggregated SQDs have been systematically investigated. Aggregation and disaggregation of the SQDs and the corresponding quenching and recovery of fluorescence occurs and guarantees the high-contrast sensing performance of the SQD system in complex and challenging aquatic environments. Our designed on-off-on nanoswitch holds great potential for the design of elemental quantum dot-based biosensors for the highly robust detection of analytes in the near future.