Ultrasensitive Electrochemiluminescence Biosensor with Silver Nanoclusters as a Novel Signal Probe and α-Fe2O3–Pt as an Efficient Co-reaction Accelerator for Procalcitonin Immunoassay,Analytical Chemistry

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Ultrasensitive Electrochemiluminescence Biosensor with Silver Nanoclusters as a Novel Signal Probe and α-Fe2O3–Pt as an Efficient Co-reaction Accelerator for Procalcitonin Immunoassay
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-01-03 , DOI: 10.1021/acs.analchem.2c04673
Xianzhen Song ₁ , Lu Zhao ₁ , Nuo Zhang ₁ , Lei Liu ₁ , Xiang Ren ₁ , Hongmin Ma ₁ , Xuan Kuang ₁ , Yuyang Li ₁ , Chuannan Luo ₁ , Qin Wei _{1,

2}

Affiliation

Herein, a high-efficiency biosensor based on ternary electrochemiluminescence (ECL) system was constructed for procalcitonin (PCT) detection. Specifically, silver nanoclusters (Ag NCs) with stable luminescence properties were prepared with small-molecule lipoic acid (LA) as the ligand, and its ECL emission in persulfate (S₂O₈^2–) was first reported. Meanwhile, the prepared Ag NCs possessed ligand-to-metal charge-transfer characteristics, thus transferring energy from LA to Ag⁺ for luminescence. Based on the small particle size, good biocompatibility, and molecular binding ability, Ag NCs-LA was used as an ideal luminescent probe. In addition, α-Fe₂O₃–Pt was introduced to facilitate the activation of S₂O₈^2–, thereby generating more sulfate radicals to react with the free radicals of Ag NCs to enhance ECL emission. The synergistic effect of the variable valence state of transition metals and high catalytic activity of noble metals endows α-Fe₂O₃–Pt with excellent catalytic ability for S₂O₈^2–. Importantly, the sensing mechanism was systematically demonstrated by UV–vis, fluorescence, and ECL analysis, as well as density functional theory calculations. At last, NKFRGKYKC was designed for specific immobilization of antibodies, thus releasing the antigen binding sites to improve the antigen recognition efficiency. Based on this, the developed biosensor showed high sensitivity for PCT detection, with a wide linear range (10 fg/mL–100 ng/mL) and a low detection limit (3.56 fg/mL), which could be extended to clinical detection of multiple biomarkers.

中文翻译：

以银纳米团簇作为新型信号探针和 α-Fe2O3-Pt 作为降钙素原免疫测定的高效共反应加速剂的超灵敏电化学发光生物传感器

在此，构建了一种基于三元电化学发光（ECL）系统的高效生物传感器，用于检测降钙素原（PCT）。具体而言，以小分子硫辛酸 (LA) 为配体制备了具有稳定发光性能的银纳米团簇 (Ag NCs)，并首次报道了其在过硫酸盐 (S 2 O 8 2– )中_的ECL_发射^。同时，所制备的 Ag NCs 具有配体到金属的电荷转移特性，从而将能量从 LA 转移到 Ag ⁺以进行发光。基于粒径小、良好的生物相容性和分子结合能力，Ag NCs-LA被用作理想的发光探针。此外，α-Fe ₂ O ₃_{–Pt 的引入促进了 S 2} O ₈^2–的活化，从而产生更多的硫酸根与 Ag NCs 的自由基反应，增强 ECL 发射。过渡金属的可变价态和贵金属的高催化活性的协同作用赋予了α-Fe ₂ O ₃ –Pt对S ₂ O ₈^{2–优异的催化能力}. 重要的是，通过紫外-可见、荧光和 ECL 分析以及密度泛函理论计算系统地证明了传感机制。最后，NKFRGKYKC被设计用于特异性固定抗体，从而释放抗原结合位点以提高抗原识别效率。基于此，开发的生物传感器对 PCT 检测具有高灵敏度，具有宽线性范围（10 fg/mL–100 ng/mL）和低检测限（3.56 fg/mL），可扩展到临床检测多种生物标志物。

更新日期：2023-01-03

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