Highly Efficient Electrochemiluminescence of MnS:CdS@ZnS Core-Shell Quantum Dots for Ultrasensitive Detection of MicroRNA.

In this work, a novel electrochemiluminescence (ECL) biosensor was developed for ultrasensitive detection of microRNA let-7a (miRNA let-7a) based on MnS:CdS@ZnS core-shell quantum dots (QDs) as ECL luminophores with high ECL efficiency. Impressively, compared to the CdS:Mn@ZnS QDs prepared by ionic doping with ECL efficiency of 0.87%, MnS:CdS@ZnS QDs synthesized by bimetallic clusters (Cd2Mn2O4) doping exhibited high ECL efficiency of up to 15.84% with S2O82- as cathodic coreactant due to the elimination of the dopants size mismatch and "self-purification" effect, which could achieve the surface defect passivation of MnS:CdS@ZnS QDs for effectively improving the ECL emission. Furthermore, with the help of strand displacement amplification (SDA), the trace target miRNA let-7a was able to be converted to a number of output DNA labeled with ferrocene (Fc) to construct an ultrasensitive ECL biosensor. The well-designed ECL biosensor for miRNA let-7a exhibited high stability and excellent sensitivity of a concentration variation from 10 aM to 1 nM and a low detection limit of 4.1 aM, which was further applied to the analysis of miRNA let-7a from cancer cell (MCF-7) lysate. Thus, this strategy provides a novel method to prepare high-efficient ECL emitters for the construction of ECL biosensing platforms in biological fields and clinical diagnosis.