College of Environmental Science & Engineering, State Key Laboratory of Pollution Control and Resource Reuse Study, Tongji University, 1239 Siping Road, Shanghai 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China; Graduate School of Life and Environmental Sciences, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8572, Japan.
College of Environmental Science & Engineering, State Key Laboratory of Pollution Control and Resource Reuse Study, Tongji University, 1239 Siping Road, Shanghai 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
Environ Int. 2019 Apr;125:135-141. doi: 10.1016/j.envint.2019.01.033. Epub 2019 Feb 1.
The development of a feasible antibiotic detection method is important in water quality analysis. In this study, we developed a metal-organic framework (MOF)-aptamer-3,3',5,5'-tetramethylbenzidine (TMB)-HO-based sensing platform composed of the reaction variable of TMB catalytic oxidation as the label (from colorless to blue) and aptamer as the target recognition element for antibiotic detection. The platform works by calculating the relation between the antibiotic concentration and the resultant decrease in MOF's catalytic activity. Basing from the comparison of typical iron-based MOF materials (Fe-MIL-53, Fe-MIL-88A, and Fe-MIL-100), we selected Fe-MIL-53 to obtain an improved signal amplification effect. The outstanding performance of the Fe-MIL-53-based sensing platform can be attributed to its topological flexibility and small electron transfer impedance. In addition, a signal increment of up to 86% was obtained with an intensified gold nanoparticle (AuNP)-supported aptamer. The inhibitory catalytic activity stemmed from the coating of antibiotic-(AuNP-aptamer) conjugates onto the outer surface of the MOF material, which increased the impedance and decreased the electron transfer efficiency. Validation results indicated that the platform showed high selectivity and sensitivity (i.e., wide linearity range of 50-200 nM, detection limit up to 8.1 ng/mL, and recovery rate of 106%-110%) for chloramphenicol detection and universal applicability for other antibiotics, including ampicillin, tetracycline, and oxytetracycline. In general, the detection reliability and easy operation of this platform render it a promising candidate for antibiotic detection in future water quality monitoring practices.
开发可行的抗生素检测方法在水质分析中很重要。在本研究中，我们开发了一种基于金属有机骨架（MOF）-适配体-3,3',5,5'-四甲基联苯胺（TMB）-HO 的传感平台，该平台的反应变量为 TMB 催化氧化（从无色变为蓝色），适配体作为抗生素检测的目标识别元件。该平台通过计算抗生素浓度与 MOF 催化活性降低之间的关系来工作。通过比较典型的铁基 MOF 材料（Fe-MIL-53、Fe-MIL-88A 和 Fe-MIL-100），我们选择了 Fe-MIL-53 以获得更好的信号放大效果。Fe-MIL-53 基传感平台的出色性能归因于其拓扑灵活性和小的电子转移阻抗。此外，通过增强金纳米粒子（AuNP）支持的适配体，获得了高达 86%的信号增量。抑制催化活性源于抗生素-（AuNP-适配体）缀合物覆盖在 MOF 材料的外表面，这增加了阻抗并降低了电子转移效率。验证结果表明，该平台对氯霉素检测具有高选择性和灵敏度（即 50-200 nM 的宽线性范围、检测限低至 8.1 ng/mL 以及回收率为 106%-110%），并且对其他抗生素（包括氨苄西林、四环素和土霉素）具有普遍适用性。总的来说，该平台的检测可靠性和易于操作使其成为未来水质监测实践中抗生素检测的有前途的候选者。
