结合基于金属-有机框架 (MOF) 的纳米酶和 G-四链体 (G4)-脱氧核糖核酸酶的高效生物传感系统,Analytical Chemistry

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结合基于金属-有机框架 (MOF) 的纳米酶和 G-四链体 (G4)-脱氧核糖核酸酶的高效生物传感系统
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-05-13 , DOI: 10.1021/acs.analchem.2c00600
Xuanxiang Mao ₁ , Fangni He ₁ , Dehui Qiu ₁ , Shijiong Wei ₁ , Rengan Luo ₁ , Yun Chen ₁ , Xiaobo Zhang ₁ , Jianping Lei ₁ , David Monchaud ₂ , Jean-Louis Mergny _{1,

3} , Huangxian Ju ₁ , Jun Zhou ₁

Affiliation

在为生物传感应用开发新的生物催化系统时，与稳健的化学结构相关的高催化效率是最终目标之一。为了更接近这些目标，我们在此报告了基于金属有机框架 (MOF) 的纳米酶和称为 G4-DNAzyme 的基于 G-四链体 (G4) 的催化系统的组合。这种方法旨在结合双方的优势（主要是前者的稳健性和后者的模块化）。为此，我们使用 MIL-53(Fe) MOF 并将其与 G4 形成序列 (F3TC) 共价连接，该序列本身与其辅因子 hemin 共价连接。所得复合物（称为 MIL-53(Fe)/G4-hemin）表现出出色的过氧化物酶模拟氧化活性和出色的稳定性（在水中储存数周）。这些特性被用来设计一种新的生物传感系统，该系统基于由纳米酶（ABTS 氧化）和一种酶——碱性磷酸酶（或 ALP，抗坏血酸 2-磷酸去磷酸化）催化的级联反应。后者毒化前者的产物，因此我们设计了一种用于 ALP（骨病和癌症的标志物）的生物传感器，检测限非常低（LOD，0.02 UL^–1 )，适用于人体血浆样本。

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Efficient Biocatalytic System for Biosensing by Combining Metal–Organic Framework (MOF)-Based Nanozymes and G-Quadruplex (G4)-DNAzymes

A high catalytic efficiency associated with a robust chemical structure are among the ultimate goals when developing new biocatalytic systems for biosensing applications. To get ever closer to these goals, we report here on a combination of metal–organic framework (MOF)-based nanozymes and a G-quadruplex (G4)-based catalytic system known as G4-DNAzyme. This approach aims at combining the advantages of both partners (chiefly, the robustness of the former and the modularity of the latter). To this end, we used MIL-53(Fe) MOF and linked it covalently to a G4-forming sequence (F3TC), itself covalently linked to its cofactor hemin. The resulting complex (referred to as MIL-53(Fe)/G4-hemin) exhibited exquisite peroxidase-mimicking oxidation activity and an excellent robustness (being stored in water for weeks). These properties were exploited to devise a new biosensing system based on a cascade of reactions catalyzed by the nanozyme (ABTS oxidation) and an enzyme, the alkaline phosphatase (or ALP, ascorbic acid 2-phosphate dephosphorylation). The product of the latter poisoning the former, we thus designed a biosensor for ALP (a marker of bone diseases and cancers), with a very low limit of detection (LOD, 0.02 U L^–1), which is operative in human plasma samples.

更新日期：2022-05-13

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