Target-induced structure-switching DNA hairpins for sensitive electrochemical monitoring of mercury (II)

Abstract

A simple, sensitive and reusable electrochemical sensor was designed for determination of mercury (II) (Hg2+) by coupling target-induced conformational switch of DNA hairpins with thymine–Hg2+–thymine (T–Hg2+–T) coordination chemistry. The hairpin probe consisted of a stem of 6 base pairs enclosing a 14 nucleotide (nt) loop and an additional 12 nt sticky end at the 3′ end. Each hairpin was labeled with ferrocene (Fc) redox tag in the middle of the loop, which was immobilized on the electrode via self-assembly of the terminal thiol moiety at the 5′ end. In the presence of target analyte, Hg2+-mediated base pairs induced the conformational change from the sticky end to open the hairpins, resulting in the ferrocene tags close to the electrode for the increasing redox current. The strong coordination reaction of T–Hg2+–T resulted in a good repeatability and intermediate precision down to 10%. The dynamic concentration range spanned from 5.0nM to 1.0μM Hg2+ with a detection limit of 2.5nM at the 3sblank level. The strategy afforded exquisite selectivity for Hg2+ against other environmentally related metal ions. Inspiringly, the developed sensor could be reused by introduction of iodide (I−).