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基于单发射体和单共反应物的双势比率电化学发光用于灵敏检测癌胚抗原。

Dual-potential ratiometric electrochemiluminescence based on single emitter and single coreactant for the sensitive detection of carcinoembryonic antigen.

机构信息

Department of Chemistry, Liaocheng University, Liaocheng, Shandong, 252059, PR China.

Department of Chemistry, Liaocheng University, Liaocheng, Shandong, 252059, PR China.

出版信息

Talanta. 2024 Jul 1;274:126023. doi: 10.1016/j.talanta.2024.126023. Epub 2024 Apr 1.

Abstract

Dual-potential ratiometric electrochemiluminescence (ECL) is in favor of resistance to environmental interference. However, two kinds of emitters or coreactants, and a wide scan potential range (>2 V) are mandatory. This work developed a new dual-potential ratiometric ECL sensor for detection of carcinoembryonic antigen (CEA) using single emitter (luminol) and single coreactant (HO) with a mild potential range from -0.1 to 0.6 V. Luminol could produce a strong cathodic ECL (E) induced by hydroxyl radicals (HO‧) from the reduction of HO, and a relatively weak anodic ECL (E). After the ferrocene modified CEA aptamer (Apt-Fc) was attached, Fc could promote E by catalyzing the oxidation of HO, and reduce E by consuming HO‧. With the cycling amplification of the exonuclease I, CEA could substantially reduce the amount of Apt-Fc, resulting in the decrease of E and the rise of E. So, the ratio of E to E (E/E) was used as the detection signal, realizing the sensitive determination of CEA from 0.1 pg mL to 10 ng mL with a LOD of 41.85 fg mL (S/N = 3). The developed sensor demonstrated excellent specificity, stability and reproducibility, with satisfactory results in practical detection.

摘要

双电位比率电化学发光(ECL)有利于抵抗环境干扰。然而,需要两种发射器或共反应物,以及宽的扫描电位范围(>2 V)。本工作开发了一种新的双电位比率 ECL 传感器,用于检测癌胚抗原(CEA),使用单一发射器(鲁米诺)和单一共反应物(HO),电位范围温和,从-0.1 到 0.6 V。鲁米诺可以通过还原 HO 产生强的阴极 ECL(E),由羟基自由基(HO‧)诱导,并且可以产生较弱的阳极 ECL(E)。在修饰了二茂铁的 CEA 适体(Apt-Fc)被连接后,Fc 可以通过催化 HO 的氧化来促进 E,并且通过消耗 HO‧来还原 E。随着外切酶 I 的循环扩增,CEA 可以大大减少 Apt-Fc 的数量,导致 E 的减少和 E 的增加。因此,E 与 E 的比值(E/E)被用作检测信号,实现了对 CEA 的灵敏检测,从 0.1 pg mL 到 10 ng mL,检出限为 41.85 fg mL(S/N = 3)。所开发的传感器表现出优异的特异性、稳定性和重现性,在实际检测中取得了令人满意的结果。

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