Regulation of Ru(bpy)₃²⁺ Electrochemiluminescence Based on Distance-Dependent Electron Transfer of Ferrocene for Dual-Signal Readout Detection of Aflatoxin B1 with High Sensitivity

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Ferrocene (Fc) is a common quencher of Ru(bpy) 3 2+ luminescence. However, interactions between Fc and Ru(bpy) 3 2+ can be extremely complicated. In this work, we reported the first use of Fc to regulate the electrochemiluminescence (ECL) of Ru(bpy) 3 2+ by tuning the length of the DNA sequence between Fc and the luminophore of nitrogen-doped graphene quantum dots-Ru(bpy) 3 2+ -doped silica nanoparticles (SiO 2 @Ru-NGQDs). The ECL of SiO 2 @Ru-NGQDs was depressed when the distance between Ru(bpy) 3 2+ and Fc was less than 8 nm; a stronger ECL was observed when the distance was more than 12 nm. The switching of the ECL of Ru(bpy) 3 2+ by Fc was attributed to the electron transfer mechanism, in which Fc participated in the redox of Ru(bpy) 3 2+ for “signal-off” ECL; this favored electron transfer at the electrode fabricated with an Fc-labeled aptamer (Fc-apt) and SiO 2 @Ru-NGQDs for “signal-on” ECL depending on the length of the DNA sequence. Here, a dual-signal readout aptasensor for aflatoxin B1 (AFB1) detection was developed via the enhanced ECL of SiO 2 @Ru-NGQDs by Fc-apt. The redox currents of Fc and the ECL of Ru(bpy) 3 2+ were simultaneously collected as yardsticks, and both decreased with higher concentrations of AFB1. The aptasensor allowed linear ranges of 3 × 10 –5 to 1 × 10 2 ng mL –1 for ECL mode and 1 × 10 –3 to 3 × 10 3 ng mL –1 for electrochemical mode. Our work provides insight into the interactions between Fc and Ru(bpy) 3 2+ . The dual-signal readout strategy is a potential platform for the versatile design of aptasensors.