Zero-Background Dual-Mode Closed Bipolar Electrode Electrochemiluminescence Biosensor Based on ZnCoN-C Potential Regulation for Ultrasensitive Detection of Ochratoxin A.

In this work, the relationship between electrochemiluminescence (ECL) signal and driving voltage was first studied by self-made reduced and oxidized closed bipolar electrodes (CBPEs). It was found that when the driving voltage was large enough, the maximum ECL signals for the two kinds of CBPEs were the same but their required drive voltages were different. Zinc cobalt nitrogen doped carbon material (ZnCoN-C) had an outstanding electric double layer (EDL) property and conductivity. Therefore, it could significantly reduce the driving voltage of two kinds of CBPE systems, reaching the maximum ECL signal of Ru(bpy). Interestingly, when the ZnCoN-C modified electrode reached the maximum ECL signal, the bare electrode signal was zero. As a proof-of-concept application, a zero-background dual-mode CBPE-ECL biosensor was constructed for the ultrasensitive detection of ochratoxin A (OTA) in beer. Considering that beer samples contained a large number of reducing substances, a reduced CBPE system was selected to build the biosensor. Furthermore, a convenient ECL imaging platform using a smartphone was built for the detection of OTA. This work used a unique EDL material ZnCoN-C to regulate the driving voltage of CBPE for the first time; thus, a novel zero-background ECL sensor was constructed. Further, this work provided a deeper understanding of the CBPE-ECL system and opened a new door for zero-background detection.