Cathode-Anode Spatial Division Photoelectrochemical Platform Based on a One-Step DNA Walker for Monitoring of...

Photoelectrochemical (PEC) biosensors carried out the whole reaction process in the same solution, which would limit the sensitivity and selectivity of detection in the sensing system. Herein, we reported a promising new cathode-anode spatial division PEC platform based on the two-electrode synergistic enhancement strategy. With the photoanode and photocathode integrated in the same current circuit, the platform exhibited an increased photocurrent response, as well as an improved anti-interference ability led by separating the two electrodes spatially. In this proposal, red light-driven AgInS₂ nanoparticles (NPs) served as the photoanode to build biometric steps and amplify the signal, whereas p-type PbS quantum dots were selected as the photocathode to increase the signal. With the participation of alkaline phosphatase (ALP) labeled on Au NPs-DNA, ascorbic acid 2-phosphate was catalyzed to produce ascorbic acid as an electron donor, resulting in the enhancement of the PEC signal. Interestingly, in the presence of miRNA-21 and T7 Exo, the one-step DNA walker amplification can be triggered to reduce the PEC signal by releasing ALP-Au NP-DNA. The constructed PEC biosensor exhibited a detection limit of as low as 3.4 fM for miRNA-21, which was expected to be applied to early clinical diagnosis. Also, we believe that the proposed cathode-anode spatial division PEC platform can open up a new view for the establishment of other types of PEC biosensors.