The authors herein described a time-gated fluorescence resonance energy transfer (TGFRET) sensing strategy employing water-soluble long lifetime fluorescence quantum dots and gold nanoparticles to detect trace Hg(2+) ions in aqueous solution. The water-soluble long lifetime fluorescence quantum dots and gold nanoparticles were functionalized by two complementary ssDNA, except for four deliberately designed T-T mismatches. The quantum dot acted as the energy-transfer donor, and the gold nanoparticle acted as the energy-transfer acceptor. When Hg(2+) ions were present in the aqueous solution, DNA hybridization will occur because of the formation of T-Hg(2+)-T complexes. As a result, the quantum dots and gold nanoparticles are brought into close proximity, which made the energy transfer occur from quantum dots to gold nanoparticles, leading to the fluorescence intensity of quantum dots to decrease obviously. The decrement fluorescence intensity is proportional to the concentration of Hg(2+) ions. Under the optimum conditions, the sensing system exhibits the same liner range from 1 × 10(-9) to 1 × 10(-8) M for Hg(2+) ions, with the detection limits of 0.49 nM in buffer and 0.87 nM in tap water samples. This sensor was also used to detect Hg(2+) ions from samples of tap water, river water, and lake water spiked with Hg(2+) ions, and the results showed good agreement with the found values determined by an atomic fluorescence spectrometer. In comparison to some reported colorimetric and fluorescent sensors, the proposed method displays the advantage of higher sensitivity. The TGFRET sensor also exhibits excellent selectivity and can provide promising potential for Hg(2+) ion detection.
An ultrasensitive "turn-on" fluorescent sensor was presented for determination of Hg(2+). 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 Hg(2+) in the sample solution, strands A and B could form hybrid structures, resulting in the fluorescence of Mn:CdS/ZnS being decreased sharply. When Hg(2+) is present in the sample solution, Hg(2+)-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 Hg(2+). The sensor exhibits two linear response ranges between fluorescence intensity and Hg(2+) 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 Hg(2+) even with interference by high concentrations of other metal ions. This sensor is successfully applied to determination of Hg(2+) 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.
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