<p>An electrochemical biosensor using gold nanoparticles (AuNPs)-doped bimetallic-organic framework (BMOF) with enhanced peroxidase-like activity was constructed to detect <i>Salmonella Typhimurium</i> (<i>S. typhimurium</i>). The BMOF of CuZr-MOF was synthesized via a&#xa0;two-step method and used as carrier to in situ immobilize AuNPs. Due to the stability of Zr-MOF, the good electrocatalytic ability of Cu (II), and the synergetic effects of AuNPs, Cu (II) and Zr (IV), the prepared AuNPs@CuZr-MOF nanozyme showed improved stability and catalytic activity to H<sub>2</sub>O<sub>2</sub> oxidation. The oxidation reaction was found to be a surface-controlled process of electron transfer and a pH-dependent electron transfer process of oxidation reaction involving two electrons. Further, AuNPs@CuZr-MOF was biofunctionalized with signal DNA probe, forming sDNA-AuNPs@CuZr-MOF nanotags. The biosensing platform was constructed on a glassy carbon electrode modified sequentially with electrodeposited AuNPs, capture DNA probe (cDNA), and BSA. Finally, a sandwich-type detection structure was formed by hybridization reactions between cDNA and target <i>invA</i> gene of <i>S. typhimurium</i>, as well as between <i>invA</i> gene and the sDNA of sDNA@AuNPs@CuZr-MOF nanotags. Under optimized experimental conditions, the biosensor achieved a linear range of 1 × 10<sup>−16</sup> to 1 × 10<sup>−8</sup> mol L<sup>−1</sup> for the target <i>invA</i> gene with a detection limit (LOD) of 6.2 × 10<sup>−17</sup> mol L<sup>−1</sup> using differential pulse voltammetry measurement (DPV). It was successfully applied to the direct and quantitative detection of <i>invA</i> gene segments in total DNA extracts of <i>S. typhimurium</i>, showing a linear range from 3.5 to 3.5 × 10<sup>6</sup>&#xa0;CFU&#xa0;mL<sup>−1</sup> and a LOD of 0.82&#xa0;CFU&#xa0;mL<sup>−1</sup>. The fabricated biosensor exhibited good selectivity, reproducibility, and storage stability, enabling its use for the detection of <i>invA</i> gene segments in contaminated milk, with recoveries between 95.9% and 103.1%.</p> Graphical Abstract <p></p>

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Electrochemical detection of S. typhimurium based on peroxidase-like activity of gold nanoparticle-doped CuZr-MOF nanozyme

  • Xiaodong Cao,
  • Chenlu Zhang,
  • Yunan Xu,
  • Wei Wang,
  • Huiying Hu,
  • Keji Chen,
  • Jing Yang,
  • Shudong He,
  • Hanju Sun,
  • Yongkang Ye

摘要

An electrochemical biosensor using gold nanoparticles (AuNPs)-doped bimetallic-organic framework (BMOF) with enhanced peroxidase-like activity was constructed to detect Salmonella Typhimurium (S. typhimurium). The BMOF of CuZr-MOF was synthesized via a two-step method and used as carrier to in situ immobilize AuNPs. Due to the stability of Zr-MOF, the good electrocatalytic ability of Cu (II), and the synergetic effects of AuNPs, Cu (II) and Zr (IV), the prepared AuNPs@CuZr-MOF nanozyme showed improved stability and catalytic activity to H2O2 oxidation. The oxidation reaction was found to be a surface-controlled process of electron transfer and a pH-dependent electron transfer process of oxidation reaction involving two electrons. Further, AuNPs@CuZr-MOF was biofunctionalized with signal DNA probe, forming sDNA-AuNPs@CuZr-MOF nanotags. The biosensing platform was constructed on a glassy carbon electrode modified sequentially with electrodeposited AuNPs, capture DNA probe (cDNA), and BSA. Finally, a sandwich-type detection structure was formed by hybridization reactions between cDNA and target invA gene of S. typhimurium, as well as between invA gene and the sDNA of sDNA@AuNPs@CuZr-MOF nanotags. Under optimized experimental conditions, the biosensor achieved a linear range of 1 × 10−16 to 1 × 10−8 mol L−1 for the target invA gene with a detection limit (LOD) of 6.2 × 10−17 mol L−1 using differential pulse voltammetry measurement (DPV). It was successfully applied to the direct and quantitative detection of invA gene segments in total DNA extracts of S. typhimurium, showing a linear range from 3.5 to 3.5 × 106 CFU mL−1 and a LOD of 0.82 CFU mL−1. The fabricated biosensor exhibited good selectivity, reproducibility, and storage stability, enabling its use for the detection of invA gene segments in contaminated milk, with recoveries between 95.9% and 103.1%.

Graphical Abstract