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基于 Fe-MOGs 的酶模拟物及其介导的电致化学发光用于从 Hela 细胞原位检测释放的 HO。

Fe-MOGs-based enzyme mimetic and its mediated electrochemiluminescence for in situ detection of HO released from Hela cells.

机构信息

School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.

School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.

出版信息

Biosens Bioelectron. 2021 Jul 15;184:113216. doi: 10.1016/j.bios.2021.113216. Epub 2021 Apr 14.

Abstract

Enzyme mimetics have attracted wide interest due to their inherent enzyme-like activity and unique physicochemical properties, as well as promising applications in disease diagnosis, treatment and monitoring. Inspired by the attributes of nonheme iron enzymes, synthetic models were designed to mimic their capability and investigate the catalytic mechanisms. Herein, metal-organic gels (Fe-MOGs) with horseradish peroxidase (HRP) like Fe-N structure were successfully synthesized though the coordination between iron and 1,10-phenanthroline-2,9-dicarboxylic acid (PDA) and exhibited excellent peroxidase-like activity. Its structure-activity relationship and the in-situ electrochemiluminescence (ECL) detection of HO secreted by Hela cells were further investigated. The highly dispersed Fe-N active sites inside Fe-MOGs were able to catalyze the decomposition of HO into large amounts of reactive oxygen species (ROS) via a Fenton-like reaction under a low overpotential. Due to the accumulation of ROS free radicals, the luminol ECL emission was significantly amplified. A proof-of-concept biosensor was constructed with a detection limit as low as 2.2 nM and a wide linear range from 0.01 to 40 μM. As a novel metal organic gels based enzyme mimetic, Fe-MOGs show great promises in early cancer detection and pathological process monitoring.

摘要

由于其固有酶样活性和独特的物理化学性质,以及在疾病诊断、治疗和监测方面的应用前景广阔,酶模拟物引起了广泛的关注。受非血红素铁酶属性的启发,设计了合成模型来模拟其能力并研究催化机制。本文通过铁与 1,10-菲啰啉-2,9-二羧酸(PDA)的配位,成功合成了具有辣根过氧化物酶(HRP)样 Fe-N 结构的金属-有机凝胶(Fe-MOGs),并表现出优异的过氧化物酶样活性。进一步研究了其结构-活性关系以及对 Hela 细胞分泌的 HO 的原位电化学发光(ECL)检测。在低过电势下,Fe-MOGs 内高度分散的 Fe-N 活性位点能够通过类芬顿反应将 HO 分解为大量活性氧(ROS)。由于 ROS 自由基的积累,鲁米诺的 ECL 发射得到了显著增强。构建了一种基于新型金属有机凝胶的酶模拟物的概念验证生物传感器,检测限低至 2.2 nM,线性范围从 0.01 到 40 μM。作为一种新型的基于金属有机凝胶的酶模拟物,Fe-MOGs 在早期癌症检测和病理过程监测方面具有广阔的应用前景。

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