Plasmon-Boosted Fe, Co Dual Single-Atom Catalysts for Ultrasensitive Luminol-Dissolved O2 Electrochemiluminescence Detection of Prostate-Specific Antigen

Abstract

Improving the sensitivity of electrochemiluminescence (ECL) systems is highly desired for in vitro ECL diagnosis and bio-detections due to the often-low content of biomarkers in diseases. And dissolved O2 (DO) as a co-reactant is considered superior to H2O2 in the most commonly used luminol ECL systems due to better stability and low biotoxicity, but it still suffers from low ECL performance due to the low reactivity of DO. In this study, an efficient luminol-DO ECL system was developed through the complexing of Fe, Co dual single-atom catalysts (D-SACs) supported by N-doped graphene with the luminol-capped Ag nanoparticles (AgNPs). Benefiting from the electronic interaction between Fe and Co metal sites in the relevant D-SACs and plasmon enhancement of AgNPs, the performance of the corresponding ECL system could be significantly boosted up to ≈677-fold under optimal testing conditions, comparable to the classic luminol-O2 system. Furthermore, the developed luminol-DO ECL system was successfully applied for the stable ultrasensitive detection of prostate-specific antigen (PSA) in a wide linear range of 1 fg/mL to 1 μg/mL, with a low limit of detection (0.98 fg/mL).