A spatial-potential resolved bipolar electrode electrochemiluminescence biosensor based on polarity conversion for...

In this work, a spatial-potential resolved bipolar electrode electrochemiluminescence (BPE-ECL) biosensor based on polarity conversion strategy and CuHCF electrocatalyst was constructed for dual-mode detection of miRNA-122 and carcinoembryonic antigen (CEA). ECL technology was firstly used to systematically study the polarity conversion of BPE. It was found that changing the polarity of the driving voltage would cause the polarity change of BPE, and led to the change of the luminescent position of Ru(bpy)₃²⁺. As a "proof-of-concept application", we developed a shielded dual-channel BPE-ECL biosensor for dual-mode detection of miRNA-122 and CEA. In order to further improve the detection sensitivity, a non-precious metal electrocatalyst CuHCF with outstanding electrocatalytic reduction activity of H₂O₂ was firstly introduced to the BPE-ECL biosensor for signal amplification, which could generate high faradaic current under the excitation of negative potential. Based on the charge neutrality principle of BPE, the enhancement of the faradaic current resulted in the ECL signal amplification of Ru(bpy)₃²⁺. The targets in the sensing grooves caused the introduction or fall off of CuHCF, which led to the ECL signal change of Ru(bpy)₃²⁺ in the signal grooves, and realized the dual-mode detection of miRNA-122 and CEA. This work provided a deeper understanding of the polarity change of BPE. Furthermore, the introduction of non-precious metal electrocatalyst had broadened the application range of BPE-ECL sensors.