Integration of Biofuel Cell-Based Self-Powered Biosensing and Homogeneous Electrochemical Strategy for Ultrasensitive and Easy-To-Use Bioassays of MicroRNA

Biofuel cell (BFC)-based self-powered biosensors have attracted substantial attentions because of their unique merits such as having no need for power sources (only two electrodes are needed). More importantly, in case it can also work in a homogeneous system, more efficient and easy-to-use bioassays could come true. Thus, herein, we proposed a novel homogeneous self-powered biosensing strategy via the integration of BFCs and a homogeneous electrochemical method, which was further utilized for ultrasensitive microRNA (miRNA) detection. To construct such an assay protocol, the cathodic electron acceptor [Fe(CN)6]3- was entrapped in the pores of positively charged mesoporous silica nanoparticles and capped by the biogate DNAs. Once the target miRNA existed, it would trigger the controlled release of [Fe(CN)6]3-, leading to the dramatic increase of the open circuit voltage. Consequently, the "signal-on" homogeneous self-powered biosensor for the ultrasensitive miRNA assay was realized. Encouragingly, the limit of detection for the miRNA-21 assay was down to 2.7 aM (S/N = 3), obviously superior to those of other analogous reported approaches. This work not only provides an ingenious idea to construct the ultrasensitive and easy-to-use bioassays of miRNA but also exhibits a successful prototype of a portable and on-site biomedical sensor.