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Exogenous Coreactant-Free Electrocatalytic Reactive Oxygen Species-Driven Dual-Signal Molecularly Imprinted
Yongqiang Li1, Kaida Kuang1, Yang Chen1
1The Education Ministry Key Lab of Resource Chemistry, Joint International Research Laboratory of Resource Chemistry, Ministry of Education, Shanghai Frontiers Science Center of Biomimetic Catalysis, Shanghai Key Laboratory of Rare Earth Functional Materials, College of Chemistry and Materials Science, Shanghai Normal University, Shanghai 200234, China.
Abstract:
Conventional dual-signal electrochemiluminescence (ECL) sensors feature high sensitivity and reliability, but the involvement of coreactants inevitably results in a complex configuration and shows reproducibility risk. Here, we propose an exogenous coreactant-free dual-signal platform, comprising luminol (anodic luminophore), CdSe quantum dots (cathodic luminophore), and Co3O4/Ti3C2 electrocatalyst (coreaction promoter). At different redox potentials, Co3O4/Ti3C2 induces water oxidation and oxygen reduction to produce •OH and O2•- radicals, which subsequently drive cathodic and anodic ECL emission, respectively. The dual-signal ECL pathways are confirmed by reactive oxygen species (ROS) scavenging, and the effect of dissolved oxygen is excluded. By integrating with molecular imprinting technology, this dual-signal ECL sensor is employed for the quantitative detection of trenbolone. It exhibits high sensitivity, broad linear range (1.0 × 101 to 1.0 × 108 fg mL-1), low detection limit, and detection capability of real samples. This work presents a new endogenous ROS-driven dual-signal ECL sensor that excludes the use of exogenous coreactants and offers new insights into ROS generation in a coreactant-free sensor design.
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