"Turn-on" fluorescent sensor for Hg2+ based on single-stranded DNA functionalized Mn:CdS/ZnS quantum dots and gold nanoparticles by time-gated mode

Abstract

An ultrasensitive "turn-on" fluorescent sensor was presented for determination of Hg2+. This method is mainly based on Hg 2+-induced conformational change of a thymine-rich single-stranded DNA. The water-soluble long-lifetime fluorescence quantum dot (Mn:CdS/ZnS) acted as the fluorophore, which was labeled on a 33-mer thymine-rich single-stranded DNA (strand A). The gold nanoparticles (GNPs) functionalized 10-mer single-stranded DNA (strand B) is selected as the quencher to quench the fluorescence of Mn:CdS/ZnS. Without Hg2+ in the sample solution, strands A and B could form hybrid structures, resulting in the fluorescence of Mn:CdS/ZnS being decreased sharply. When Hg2+ is present in the sample solution, Hg2+-mediated base pairs induced the folding of strand A into a hairpin structure, leading to the release of GNPs-tagged strand B from the hybrid structures. The fluorescence signal is then increased obviously compared with that without Hg2+. The sensor exhibits two linear response ranges between fluorescence intensity and Hg2+ concentration. Meanwhile, a detection limit of 0.18 nM is estimated based on 3α/slope. Selectivity experiments reveal that the fluorescent sensor is specific for Hg2+ even with interference by high concentrations of other metal ions. This sensor is successfully applied to determination of Hg2+ in tap water and lake water samples. This sensor offers additional advantage to efficiently reduce background noise using long-lifetime fluorescence quantum dots by a time-gated mode. With excellent sensitivity and selectivity, this sensor is potentially suitable for monitoring of Hg 2+ in environmental applications. © 2012 American Chemical Society.