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<p>Single-atom nanozymes (SANs) are emerging as interfacial catalysts that can modulate surface-confined reactive oxygen species (ROS) generation at the electrode/solution boundary. Herein, an interface-driven electrochemiluminescence (ECL) aptasensor was constructed for the ultrasensitive detection of zearalenone (ZEN), a mycotoxin of significant concern. Oxidase-mimetic Co–N/C SANs (Co-SAC@NC) immobilized on a glassy carbon electrode catalyze the reduction of dissolved O<sub>2</sub> to ·OH and O<sub>2</sub>·⁻, followed by in-situ generation of ROS, producing a 13-fold enhancement of luminol ECL without the addition of external H<sub>2</sub>O<sub>2</sub>. A ferrocene-labelled reporter DNA (Fc-DNA) tethered to the Co-SAC@NC surface quenches luminol ECL by trapping holes at the electrode interface; upon target binding, a magnetic-bead-supported HCR-CRISPR-Cas12a cascade is triggered, trans-cleaving the Fc-DNA and thus restoring the native ECL intensity. The concentration-dependent interfacial cleavage affords a linear range of 0.3–200 ng/mL and a LOD of 0.087 ng/mL (S/<i>N</i> = 3) for the determination of ZEN. This work establishes a modular interfacial amplification platform with potential for generalization by marrying SANs catalysis with a CRISPR-Cas12a/HCR nucleic acid cascade for advanced ECL bioanalysis.</p> Graphical abstract <p></p>

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Triple-amplification electrochemiluminescence aptasensor integrating single-atom nanozyme catalysis with CRISPR-Cas12a/HCR cascade for zearalenone detection

  • 期刊论文

  • 发表日期：

    2026年7月1日

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  • Huifeng Xu,
  • Xiao Hu,
  • Ronglin Chen,
  • Shufei Huang,
  • Lili Wang,
  • Lishuang Yu,
  • Xihai Li,
  • Xi Zhu

摘要

Single-atom nanozymes (SANs) are emerging as interfacial catalysts that can modulate surface-confined reactive oxygen species (ROS) generation at the electrode/solution boundary. Herein, an interface-driven electrochemiluminescence (ECL) aptasensor was constructed for the ultrasensitive detection of zearalenone (ZEN), a mycotoxin of significant concern. Oxidase-mimetic Co–N/C SANs (Co-SAC@NC) immobilized on a glassy carbon electrode catalyze the reduction of dissolved O2 to ·OH and O2·⁻, followed by in-situ generation of ROS, producing a 13-fold enhancement of luminol ECL without the addition of external H2O2. A ferrocene-labelled reporter DNA (Fc-DNA) tethered to the Co-SAC@NC surface quenches luminol ECL by trapping holes at the electrode interface; upon target binding, a magnetic-bead-supported HCR-CRISPR-Cas12a cascade is triggered, trans-cleaving the Fc-DNA and thus restoring the native ECL intensity. The concentration-dependent interfacial cleavage affords a linear range of 0.3–200 ng/mL and a LOD of 0.087 ng/mL (S/N = 3) for the determination of ZEN. This work establishes a modular interfacial amplification platform with potential for generalization by marrying SANs catalysis with a CRISPR-Cas12a/HCR nucleic acid cascade for advanced ECL bioanalysis.

Graphical abstract