Journal
ANALYTICAL CHEMISTRY
Volume 89, Issue 17, Pages 8830-8835Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.7b01251
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Funding
- NSFC [21475035, 21235002]
- Foundation for Innovative Research Groups of NSFC [21521063]
- Hunan Provincial Innovation Foundation for Postgraduate [CX2016B112]
- China Scholarship Council [201606130011]
- PCSIRT [IRT1238]
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Biomolecular receptors such as nucleic acids that switch between two or more conformations upon binding to a specific target can be used to build specific and sensitive biosensors. In this work, based on the electrochemical dual signaling ratiometric strategy and triple-helix molecular switch, we developed a selective, reusable, and simple electrochemical DNA (E-DNA) biosensor for target DNA (T-DNA) detection. A hairpin DNA capture probe labeled with methylene blue (MB-DNA) self-assembles on the surface of a gold electrode (GE) through Au-S bond, and then a single-strand DNA modified with two ferrocenes (Fc-DNA) on each end to enhance the oxidation signal hybridizes with the MB-DNA to form a triple-helix conformation. When T-DNA exists, the Fc-DNA hybridizes with T-DNA disassembling the triple-helix stem and allowing the MB-DNA to revert to its hairpin structure. Hence, the Fc tags diffuse away from the GE surface while the MB tags remain affixed close to it, resulting in a decrease in the peak current of Fc (I-Fc) and an increase in that of MB (I-MB). The linear relationship between the value of I-MB/I-Fc and the T-DNA concentration is observed from 0.5 to 80 pM, and the limit of detection is as low as 0.12 pM. The developed E-DNA biosensor may have great potential in the electrochemical detection of a wide range of analytes and be a biosensing platform for early clinical diagnosis and biomedical research.
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