Simultaneous Detection of Ovarian Cancer-Concerned HE4 and CA125 Markers Based on Cu Single-Atom-Triggered CdS QDs and Eu MOF@Isoluminol ECL

Simultaneous detection of different disease markers is significant for clinical diagnosis. In this work, a dual-signal electrochemiluminescence (ECL) immunosensor was constructed for the simultaneous detection of carbohydrate antigen 125 (CA125) and human epithelial protein 4 (HE4) markers of ovarian cancer. The results showed that the Eu metal–organic framework-loaded isoluminol–Au nanoparticles (Eu MOF@Isolu–Au NPs) could generate a strong anodic ECL signal through synergistic interaction; as cathodic luminophore, the composite of carboxyl-functionalized CdS quantum dots and N-doped porous carbon-anchored Cu single-atom catalyst could catalyze H2O2 co-reactant to produce a large amount of •OH and O2•–, making the anodic and cathodic ECL signals significantly increase and become stable. Based on the enhancement strategy, a sandwich immunosensor was constructed for the simultaneous detection of ovarian cancer-associated CA125 and HE4 markers by combining antigen–antibody specific recognition and magnetic separation technique. The resulting ECL immunosensor displayed high sensitivity, a wide linear response range of 0.005∼500 ng mL–1, and low detection limits of 0.37 and 1.58 pg mL–1 for CA125 and HE4, respectively. Furthermore, it had excellent selectivity, stability, and practicability in the detection of real serum samples. This work establishes a framework for in-depth design and application of single-atom catalysis in ECL sensing.