Abstract
A novel magnetic controlled photoelectrochemical (PEC) sensing system was designed for sensitive detection of prostate-specific antigen (PSA) using reduced graphene oxide-functionalized BiFeO3 (rGO-BiFeO3) as the photoactive material and target-triggered hybridization chain reaction (HCR) for signal amplification. Remarkably enhanced PEC performance could be obtained by using rGO-BiFeO3 as the photoelectrode material due to its accelerated charge transfer and improved the visible light absorption. Additionally, efficient and simple operation could be achieved by introducing magnetic controlled flow-through device. The assay mainly involved in anchor DNA-conjugated magnetic bead (MB-aDNA), PSA aptamer/trigger DNA (Apt-tDNA) and two glucose oxidase-labeled hairpins (H1-GOx and H2-GOx). Upon addition of target PSA, the analyte initially reacted with the aptamer to release the trigger DNA, which partially hybridized with the anchor DNA on the MB. Thereafter, the unpaired trigger DNA on the MB opened the hairpin DNA structures in sequence and propagated a chain reaction of hybridization events between two alternating hairpins to form a long nicked double-helix with numerous GOx enzymes on it. Subsequently, the enzymatic product (H2O2) generated and consumed the photo-excited electrons from rGO-BiFeO3 under visible light irradiation to enhance the photocurrent. Under optimal conditions, the magnetic controlled PEC sensing system exhibited good photocurrent responses toward target PSA within the linear range of 0.001 - 100ng/mL with a detection limit of 0.31pg/mL. Moreover, favorable selectivity, good stability and satisfactory accuracy were obtained. The excellent analytical performance suggested that the rGO-BiFeO3-based PEC sensing platform could be a promising tool for sensitive, efficient and low cost detection of PSA in disease diagnostics.