A waste-free entropy-driven DNA nanomachine for smartly designed photoelectrochemical biosensing of MicroRNA-155

DNA nanotechnology has been booming in many fields such as biosensors, logic gates, and material science. Typically, as a kind of powerful isothermal and enzyme-free DNA amplifier in biosensors, entropy-driven DNA nanomachines are superior to hairpin-based ones in speed, specificity, stability, and simplicity. However, the atomic economy of non-covalent molecular reactions in these machines is not high, and DNAs waste is typically generated during operation. Herein, in order to further save costs and improve the performance, we report a novel design for a smart photoelectrochemical (PEC) biosensor of microRNA-155 by engineering waste-free entropy-driven DNA amplifiers conjugated to superparamagnetic Fe3O4@SiO2 particles. This elegant design efficiently avoids leaving redundant DNA strands and waste complex in the amplification system, and all the displaced DNA strands can be regenerated into double-stranded structures, making the reaction irreversible. Thanks to superparamagnetic Fe3O4@SiO2 particles, this strategy is achieved by effectively enriching, extracting, and cleaning target analogs to prevent co-existing species from remaining on the modified electrode surface, enabling a highly specific and sensitive PEC biosensor. This innovative study will be a new perspective on microRNAs detection in complex biological systems, paving the way for the design of waste-free DNA molecular machines and promoting the development of DNA nanotechnology.