Tetrahedral DNA nanostructure-enabled electrochemical aptasensor for ultrasensitive detection of fumonisin B1 with extended dynamic range

Abstract

Fumonisin B1 (FB1) is common contaminant in agricultural and food products, and sensors with high sensitivity and broad dynamic range are extremely required for FB1 determination. Herein, we reported the tetrahedral DNA nanostructure (TDN)-enabled electrochemical aptasensor for FB1 detection at sub-fg mL−1 level with a dynamic range of 7-folds magnitude. TDN with side length of 5.67 nm was designed to fabricate the substrate for FB1 aptamer anchoring, aiming to achieve the controllable and stable assembly of sensing interface by tuning the assembly density of TDN; TDN at the electrode acts as the anchor for aptamer, absorption of methylene blue as signal generator. Assistant aptamer was added into the sample solution to deplete FB1, reducing the amount of free FB1, thereby extending dynamic range of sensing system. Simultaneously, the negatively-charged TDN can efficiently depress absorption of free aptamer in sample solution. In this way, the utilization of TDN helps to enable the sensor with higher sensitivity and extended dynamic range for FB1. Consequently, the developed sensor allowed a linear dynamic range of 0.500 fg mL−1~1.00 ng mL−1, while the limit of detection was offered to be 0.306 fg mL−1, which was the lowest among the available methods. The applicability of aptasensor was validated by rice sample analysis, which exhibited the comparable reliability of liquid-chromatography tandem mass spectrometry/mass spectrometry. Our work has provided an efficient sensing platform for FB1, and the strategy can be also extended to fabricate sensors for other mycotoxins.