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铜掺杂铽金属有机框架作为灵敏检测细胞角蛋白19片段的电化学发光发射体

Copper doped terbium metal organic framework as emitter for sensitive electrochemiluminescence detection of CYFRA 21-1.

作者信息

Zhou Limin, Yang Lei, Wang Chao, Jia Hongying, Xue Jingwei, Wei Qin, Ju Huangxian

机构信息

Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, China.

Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, China; State Key Laboratory of Analytical Chemistry for Life Science, College of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, China.

出版信息

Talanta. 2022 Feb 1;238(Pt 2):123047. doi: 10.1016/j.talanta.2021.123047. Epub 2021 Nov 6.

DOI:10.1016/j.talanta.2021.123047
PMID:34801904
Abstract

Lanthanide metal organic frameworks (L-MOFs) are emerging as promising electrochemiluminescence (ECL) emitters for bioanalysis. This work proposed a copper doped terbium MOF as a luminescent tag for construction of a "signal-on" ECL immunosensing method. The Tb-Cu-PA MOF was prepared using Tb and Cu ions as metal linkers and m-phthalic acid as bridge ligand, and exhibited strong ECL emission with KSO as a coreactant. The immunosensor was prepared by immobilizing capture antibody on Pd nanoparticles modified Ni-Co layered double hydroxide (Pd-ZIF-67@LDH) nanoboxes, which showed strong electrocatalytic activity toward the reduction of SO for amplifying the ECL signal. Upon the sandwich-typed immunoreactions, Tb-Cu-PA MOF labeled antibody was introduced onto the immunosensor for sensitive ECL detection of target protein. Using cytokeratin 19 fragment 21-1 (CYFRA21-1), a representative lung cancer biomarker, as target model, the ECL immunosensing method showed a linear range of 0.01-100 ng/mL and a detection limit of 2.6 pg/mL (S/N = 3). This immunosensing strategy highlighted the advances of using luminescent and electroactive MOFs in the developments of highly efficient immunosensors for bioanalysis.

摘要

镧系金属有机框架(L-MOFs)正成为用于生物分析的有前景的电化学发光(ECL)发光体。这项工作提出了一种铜掺杂的铽金属有机框架作为发光标签,用于构建一种“信号开启”的ECL免疫传感方法。以铽和铜离子作为金属连接体、间苯二甲酸作为桥连配体制备了Tb-Cu-PA金属有机框架,其以过硫酸钾作为共反应剂时表现出强烈的ECL发射。通过将捕获抗体固定在钯纳米颗粒修饰的镍钴层状双氢氧化物(Pd-ZIF-67@LDH)纳米盒上制备免疫传感器,该纳米盒对过硫酸根的还原表现出强烈的电催化活性以放大ECL信号。在夹心型免疫反应中,将Tb-Cu-PA金属有机框架标记的抗体引入免疫传感器用于对目标蛋白进行灵敏的ECL检测。以细胞角蛋白19片段21-1(CYFRA21-1),一种代表性的肺癌生物标志物,作为目标模型,该ECL免疫传感方法显示出0.01 - 100 ng/mL的线性范围和2.6 pg/mL的检测限(S/N = 3)。这种免疫传感策略突出了在开发用于生物分析的高效免疫传感器中使用发光和电活性金属有机框架的优势。

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