Ultrasensitive Electrochemiluminescence Biosensor Based on 2D Co3O4 Nanosheets as a Coreaction Accelerator and Highly Ordered Rolling DNA Nanomachine as a Signal Amplifier for the Detection of MicroRNA

A novel ultrasensitive electrochemiluminescence (ECL) biosensor was constructed using two-dimensional (2D) Co₃O₄ nanosheets as a novel coreaction accelerator of the luminol/H₂O₂ ECL system for the detection of microRNA-21 (miRNA-21). Impressively, coreaction accelerator 2D Co₃O₄ nanosheets with effective mutual conversion of the Co²⁺/Co³⁺ redox pair and abundant active sites could promote the decomposition of coreactant H₂O₂ to generate more superoxide anion radicals (O₂^•-), which reacted with luminol for significantly enhancing ECL signals. Furthermore, the trace target miRNA-21 was transformed into a large number of G-wires through the strand displacement amplification (SDA) process to self-assemble the highly ordered rolling DNA nanomachine (HORDNM), which could tremendously improve the detection sensitivity of biosensors. Hence, on the basis of the novel luminol/H₂O₂/2D Co₃O₄ nanosheet ternary ECL system, the biosensor implemented ultrasensitive detection of miRNA-21 with a detection limit as low as 4.1 aM, which provided a novel strategy to design an effective ECL emitter for ultrasensitive detection of biomarkers for early disease diagnosis.