Thermodynamic-assisted highly effective target converting strategy for sensitive electrochemical detection of trace lead (II) ion

Abstract

In the present work, a thermodynamic-assisted target-converting strategy was designed by utilizing new 2D DNA nanoprobes (DNPs) to develop electrochemical biosensors for the sensitive determination of trace Pb2+. Herein, a stable DNP with a special structure was prepared through the hybridization reaction between three single-strand DNA (RS1, RS2, and P). Once the existence of Pb2+, the DNP will crumble and then release RS1 and RS2 due to the strong thermodynamic instability of the RS1/RS2 duplex. since RS1 and RS2 were designed in the same sequence in the free domain, they can be simultaneously used as effective output DNA, enhancing the conversion rate of Pb2+to ssDNA up to 1:2. Following the same principle, ferrocene-labeled bipedal DNPs (Fc-bDNPs) are prepared for stable electrochemical signal output. In the presence of RS1, RS2, and a hairpin DNA strand (H1), the ferrocene-labeled DNA strands (S3) escape from the Fc-bDNPs due to strand-displacement reaction, accompanying release of the two ssDNA outputs that can simultaneously trigger another strand-displacement reaction. Consequently, the one Pb2+input makes multiple Fc-labeled DNA strands far away from the electrode surface, resulting in a dramatic decrease in the response current of Fc. The developed biosensors show a linear relationship between current value and logarithmic concentration of Pb2+ ranging from 1 pM to 40 nM with a detection limit of 0.30 pM.