基于具有过氧化物酶样活性的 MIL-101(Fe)-NH2,用于检测铬(Ⅵ)的荧光/比色探针。

IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Talanta Pub Date : 2024-12-01 Epub Date: 2024-08-28 DOI:10.1016/j.talanta.2024.126785
Shengyuan Zhang, Haiyan Li, Dezhi Yang, Yaling Yang
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引用次数: 0

摘要

本研究采用简单的溶热法合成了铁基金属有机框架(MIL-101(Fe)-NH2)纳米粒子,并将其用于检测 Cr(Ⅵ)。MIL-101(Fe)-NH2具有双重功能:2-氨基对苯二甲酸(NH2-BDC)配体具有强烈的荧光发射,铁金属节点能够直接促进3,3',5,5'-四甲基联苯胺(TMB)的氧化,生成氧化TMB(ox-TMB)。我们的研究结果表明,抗坏血酸(AA)等还原剂可使 MIL-101(Fe)-NH2 的结构塌缩,因为 AA 还原了 Fe3+,从而释放出 NH2-BDC。在 Cr(Ⅵ)存在的情况下,由于 Fe3+ 和 Cr(Ⅵ)的竞争性还原,MIL-101(Fe)-NH2 + AA 体系的荧光强度会降低。尽管如此,Cr(Ⅵ) 仍能显著加速 MIL-101(Fe)-NH2 对 TMB 的氧化,因为它能提高 Fe3+ 和 Fe2+ 之间的电子转移率。因此,我们开发了一种荧光/比色双模式平台,用于检测 Cr(Ⅵ),其线性范围广(7.5-750 μg/L 和 13.3-1000 μg/L),检测限低(0.99 μg/L 和 1.98 μg/L)。这种具有释放配体能力的 MOF 不仅为设计新型发光材料提供了灵感,还为检测铬(Ⅵ)提供了一种新颖可靠的解决方案。
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Fluorescent/colorimetric probe for the detection of Cr(Ⅵ) based on MIL-101(Fe)-NH2 with peroxidase-like activity.

In the present research, Fe-based metal-organic frameworks (MIL-101(Fe)-NH2) nanoparticles were synthesized by simple solvothermal methods and used to assay Cr(Ⅵ). The MIL-101(Fe)-NH2 performs dual functions: the 2-aminoterephthalic acid (NH2-BDC) ligand endows a strong fluorescence emission, and the Fe metal nodes are able to facilitate the oxidation of 3,3',5,5'- tetramethylbenzidine (TMB) directly, resulting in the generation of oxidized-TMB (ox-TMB). Our research results showed that reducing agents such as ascorbic acid (AA) can collapse the structures of MIL-101(Fe)-NH2 because of the reduction of Fe3+ by AA, resulting in release of NH2-BDC. In the presence of Cr(Ⅵ), the fluorescence intensity of the MIL-101(Fe)-NH2 + AA system will be decreased due to the competitive reduction of Fe3+ and Cr(Ⅵ). Nevertheless, Cr(Ⅵ) can significantly accelerate the oxidation of TMB by MIL-101(Fe)-NH2 as it boosts the electron transfer rate between Fe3+ and Fe2+. Therefore, a fluorescent/colorimetric dual-mode platform was developed for the detection of Cr(Ⅵ) with an extensive linear range (7.5-750 μg/L and 13.3-1000 μg/L) as well as a remarkably low detection limit (0.99 μg/L and 1.98 μg/L). This MOF with the ability to release ligands not only provides inspiration for the design of new luminescent materials, but also offers a novel and reliable solution for the detection of Cr(Ⅵ).

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来源期刊
Talanta
Talanta 化学-分析化学
CiteScore
12.30
自引率
4.90%
发文量
861
审稿时长
29 days
期刊介绍: Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.
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