Sensitive and selective detection of Hg2+ in tap and canal water via self-enhanced ECL aptasensor based on NH2–Ru@SiO2-NGQDs

TALANTA(2021)

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摘要
In the present study, a novel self-enhanced electrochemiluminescence (ECL) aptasensor which combined self-enhanced ECL composite as signal response element and aptamer as the specific recognition element was firstly proposed for the sensitive and selective detection of Hg2+. Innovatively, the luminophore Ru(bpy)32+-doped silica nanoparticles functionalized with 3-aminopropyltriethoxysilane (NH2–Ru@SiO2) and the co-reactant nitrogen doped graphene quantum dots (NGQDs) were bound together to form the self-enhanced ECL composite, NH2–Ru@SiO2-NGQDs, by electrostatic adsorption. Satisfactorily, high and stable luminous efficiency of NH2–Ru@SiO2-NGQDs was obtained benefited from the short electron transfer distance and low energy loss of self-enhanced-typal ECL composite. For the fabrication of the self-enhanced ECL aptasensor for Hg2+ detection, the Hg2+ aptamer, of which one end was connected to NH2–Ru@SiO2-NGQDs, and the other end was fixed on glass carbon electrode (GCE) surface through Au–S bond, was served as a bridge. Upon the addition of Hg2+, the aptamer was bent due to the formation of thymine-Hg2+-thymine (T-Hg2+-T) specific structure, which caused the self-enhanced ECL composite was close to the GCE surface. On this basis, a linearly enhanced ECL signal was acquired with the concentration of Hg2+ in the range of 5.0 × 10−11 M − 1.0 × 10−6 M with excellent selectivity, repeatability and stability in 3 min for each assay. In addition, the proposed aptasensor showed satisfying accuracy and practicability for Hg2+ analysis in tap and canal water verified by the inductively coupled plasma-mass spectrometry (ICP-MS) method.
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关键词
Nitrogen doped graphene quantum dots,Self-enhanced electrochemiluminescence,Aptasensor,Hg2+
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