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<p>Overcoming the critical limitation of poor sensitivity in electrochemical biosensors for early breast cancer diagnosis, an innovative approach&#xa0;is presented. We developed a robust coordination strategy, utilizing serine-functionalized graphene quantum dots (SGQDs), to synthesize Au<sub>0.1</sub>FeCoNiCu high-entropy alloy nanoparticles (HEA NPs). The resulting Au<sub>0.1</sub>FeCoNiCu HEA NPs (32 ± 1.7&#xa0;nm) exhibit single a face centered cubic (FCC) phase, good elemental homogeneity, and graphene surface modification. This unique structure confers a significantly enhanced catalytic activity (&gt; 12-fold higher than pure Au NPs) and a superior affinity towards polar electrolytes. Furthermore, these HEA NPs were integrated&#xa0;with a DNA walker circuit to construct one electrochemical biosensor for ultrasensitive detection of miRNA-21. The target miRNA-21 triggers the DNA walker process, immobilizing ferrocene molecules on the electrode surface generating a measurable electrochemical signal. This dual-amplification strategy (HEA NP catalysis + DNA walker) achieved an unprecedented sensitivity: a linear current response (at 0.22&#xa0;V) over an extraordinary range (1 × 10⁻<sup>2</sup>⁰ M to 1 × 10⁻<sup>15</sup>&#xa0;M) and a record-low detection limit of 3.4 × 10⁻<sup>21</sup>&#xa0;M. This represents 2–3 orders of magnitude sensitivity improvement over the state-of-the-art sensors, successfully demonstrated in serum analysis.</p> Graphical Abstract <p></p>

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Ultrasensitive sensing platform based on Au0.1FeCoNiCu high-entropy alloy nanoparticle-DNA walker dual signal amplification for electrochemical detection of miRNA-21

  • 期刊论文

  • 发表日期：

    2025年8月10日

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  • Li Ruiyi,
  • Li Mingyao,
  • Wang Miao,
  • Li Zaijun

摘要

Overcoming the critical limitation of poor sensitivity in electrochemical biosensors for early breast cancer diagnosis, an innovative approach is presented. We developed a robust coordination strategy, utilizing serine-functionalized graphene quantum dots (SGQDs), to synthesize Au0.1FeCoNiCu high-entropy alloy nanoparticles (HEA NPs). The resulting Au0.1FeCoNiCu HEA NPs (32 ± 1.7 nm) exhibit single a face centered cubic (FCC) phase, good elemental homogeneity, and graphene surface modification. This unique structure confers a significantly enhanced catalytic activity (> 12-fold higher than pure Au NPs) and a superior affinity towards polar electrolytes. Furthermore, these HEA NPs were integrated with a DNA walker circuit to construct one electrochemical biosensor for ultrasensitive detection of miRNA-21. The target miRNA-21 triggers the DNA walker process, immobilizing ferrocene molecules on the electrode surface generating a measurable electrochemical signal. This dual-amplification strategy (HEA NP catalysis + DNA walker) achieved an unprecedented sensitivity: a linear current response (at 0.22 V) over an extraordinary range (1 × 10⁻2⁰ M to 1 × 10⁻15 M) and a record-low detection limit of 3.4 × 10⁻21 M. This represents 2–3 orders of magnitude sensitivity improvement over the state-of-the-art sensors, successfully demonstrated in serum analysis.

Graphical Abstract