基于 Cu 单原子触发的 CdS 量子点和 Eu MOF@Isoluminol ECL 同时检测卵巢癌相关的 HE4 和 CA125 标志物,Analytical Chemistry

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基于 Cu 单原子触发的 CdS 量子点和 Eu MOF@Isoluminol ECL 同时检测卵巢癌相关的 HE4 和 CA125 标志物
Analytical Chemistry ( IF 6.7 ) Pub Date : 2023-03-03 , DOI: 10.1021/acs.analchem.3c00273
Yun Tang ₁ , Yiwei Liu ₁ , Yide Xia ₁ , Faqiong Zhao ₁ , Baizhao Zeng ₁

Affiliation

同时检测不同疾病标志物对临床诊断具有重要意义。在这项工作中，构建了双信号电化学发光 (ECL) 免疫传感器，用于同时检测卵巢癌的碳水化合物抗原 125 (CA125) 和人上皮蛋白 4 (HE4) 标记物。结果表明，载有 Eu 金属-有机骨架的异鲁米诺-Au 纳米粒子（Eu MOF@Isolu-Au NPs）可通过协同作用产生强阳极 ECL 信号；作为阴极发光体，羧基功能化的CdS量子点和N掺杂多孔碳锚定Cu单原子催化剂的复合物可以催化H ₂ O ₂共反应物产生大量的^• OH和O ₂^•–，使得阳极和阴极ECL信号显着增加并趋于稳定。基于增强策略，结合抗原抗体特异性识别和磁分离技术，构建了夹心免疫传感器，用于同时检测卵巢癌相关的 CA125 和 HE4 标志物。由此产生的 ECL 免疫传感器对 CA125 和 HE4 表现出高灵敏度、0.005∼500 ng mL ^–1的宽线性响应范围以及分别为 0.37 和 1.58 pg mL ^–1的低检测限。此外，它在实际血清样品的检测中具有优异的选择性、稳定性和实用性。这项工作为单原子催化在 ECL 传感中的深入设计和应用建立了框架。

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Simultaneous Detection of Ovarian Cancer-Concerned HE4 and CA125 Markers Based on Cu Single-Atom-Triggered CdS QDs and Eu MOF@Isoluminol ECL

Simultaneous detection of different disease markers is significant for clinical diagnosis. In this work, a dual-signal electrochemiluminescence (ECL) immunosensor was constructed for the simultaneous detection of carbohydrate antigen 125 (CA125) and human epithelial protein 4 (HE4) markers of ovarian cancer. The results showed that the Eu metal–organic framework-loaded isoluminol–Au nanoparticles (Eu MOF@Isolu–Au NPs) could generate a strong anodic ECL signal through synergistic interaction; as cathodic luminophore, the composite of carboxyl-functionalized CdS quantum dots and N-doped porous carbon-anchored Cu single-atom catalyst could catalyze H₂O₂ co-reactant to produce a large amount of ^•OH and O₂^•–, making the anodic and cathodic ECL signals significantly increase and become stable. Based on the enhancement strategy, a sandwich immunosensor was constructed for the simultaneous detection of ovarian cancer-associated CA125 and HE4 markers by combining antigen–antibody specific recognition and magnetic separation technique. The resulting ECL immunosensor displayed high sensitivity, a wide linear response range of 0.005∼500 ng mL^–1, and low detection limits of 0.37 and 1.58 pg mL^–1 for CA125 and HE4, respectively. Furthermore, it had excellent selectivity, stability, and practicability in the detection of real serum samples. This work establishes a framework for in-depth design and application of single-atom catalysis in ECL sensing.

更新日期：2023-03-03

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