A novel ratiometric electrochemical aptasensor based on M-shaped functional DNA complexes for simultaneous detection of trace lead and mercury ions in series aquatic edible vegetables

Abstract

Simultaneous quantification of multiple heavy metal ions (HMIs) is essential due to enhanced toxicity induced by synergistic effects. The currently available detection methods suffer from drawbacks such as costly devices, poor anti-interference, and specificity. In this work, a ratiometric electrochemical aptasensor for simultaneous detection of trace lead (Pb2+) and mercury ions (Hg2+) was developed. Here, a metal-organic framework, UiO-66-CNTs, with inherent and stable electrochemical signal was used for loading complementary strands (CSs) and internal reference. Guanine-rich and thymine-rich oligonucleotides, labelled with carbon dots (CDs), acted as aptamers (Apts) and hybridized with CSs to form M-shaped DNA complexes. Pb2+ and Hg2+ could be recognized and captured by Apts to form Pb2+-G-quadruplex and T-Hg2+-T complexes, leading to the destruction of M-shaped DNA complexes and changes in CDs’ signal. The current ratios, ICDs/IUiO-66-CNTs, were applied to quantify Pb2+ and Hg2+. Benefiting from the anti-interference ability of the ratiometric strategy and the specificity of Apts, the proposed method enabled detection Pb2+ and Hg2+ through simple instrumentation, with detection limits of 2.0 ng mL−1 and 0.5 ng mL−1. Moreover, it was applied to assess Pb2+ and Hg2+ contamination in series of aquatic edible vegetables. The experimental results were consistent with inductively coupled plasma-mass spectrometry (ICP-MS), demonstrating its potential in practical applications.