High-Entropy Oxide for Highly Efficient Luminol-Dissolved Oxygen Electrochemiluminescence and Biosensing Applications

The luminol-dissolved O₂ (DO) electrochemiluminescence (ECL) sensing system has recently gained growing interest; however, the drawback of the ultra-low ECL signal response greatly hinders its potential quantitative applications. In this work, for the first time, we explored the use of high entropy oxide (HEO) comprising five metal ingredients (Ni, Co, Cr, Cu, and Fe), to accelerate the reduction reaction of DO into reactive oxygen species (ROS) for boosting the ECL performance of the luminol-DO system. Benefiting from the existing abundant oxygen vacancies induced by the unique crystal structure of the HEO, DO could be efficiently converted into ROS, thus significantly boosting the performance of the corresponding ECL sensor (with an ∼240-fold signal enhancement in this study). As a proof of concept, under optimal conditions, the developed HEO-involved luminol-DO ECL sensing system was successfully applied for efficient biosensing of dopamine and alkaline phosphatase with a fine linear range from 1 pM to 10 nM and from 0.01 to 100 U/L as well as a low limit of detection of 5.2 pM and 0.008 U/L, respectively.