The Label-Free Fluorescence Detection of Inorganic and Organic Mercury Based on DNA-Templated Gold Nanoclusters

Heavy metal mercury is one of the most significant and toxic environmental contaminants. Its inorganic form (Hg²⁺) and organic form (organic mercury, OrHg) can cause irreversible harm to human health and the ecological environment, and the latter is particularly prone to bioaccumulation and bioamplification in the food chain. Therefore, there is an urgent need for a rapid, reliable and specific detection of Hg²⁺ and OrHg to evaluate the potential risk for human health. Here, a novel label-free fluorescent sensing platform based on ssDNA aptamer (A_A-T7)-templated AuNCs was established for sensitive recognition and specific detection of Hg²⁺ and OrHg. In the presence of OrHg, the fluorescence of pure A_A-T7-templated AuNCs was visibly enhanced through forming Ag/AuNCs based on Ag⁰-doped AIEE effect. However, they were obviously quenched because of generating non-fluorescent Au/Ag/Hg ANPs via metallophilic interactions among Au³⁺, Ag⁺, and Hg²⁺ (5d¹⁰-4d¹⁰-5d¹⁰) when only Hg²⁺ existed. This fluorescent sensing platform could detect as low as 20.0 nM (4.0 ng Hg/g) and has a good linear detection range, with target concentrations ranging from 0.25 μM to 2.00 μM, recoveries of 98.0-108.0%, and RSD ≤ 5.0%. Low-toxic A_A-T7-templated AuNCs could be used for cytotoxicity analysis and intracellular fluorescent imaging. The method has been successfully applied to the determination of Hg²⁺ and OrHg in tap water, seawater and dried golden pomfret fish muscle samples, demonstrating promising prospects for the assay of mercury species in environmental samples and aquatic products to ensure human health and food safety.