College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences , Peking University , Beijing 100871 , China.
Institute of Cardiovascular Disease , First Affiliated Hospital of Nanjing Medical University , Nanjing 210029 , China.
ACS Sens. 2019 Sep 27;4(9):2351-2357. doi: 10.1021/acssensors.9b00914. Epub 2019 Sep 6.
A facile strategy for in situ growing triethanolamine (TEOA)-functionalized metal-organic framework (TEOA@MOF) on the two-dimensional graphene oxide (GO) or g-CN nanosheets via the self-assembly technique was introduced. In this method, Zn was first attached on the carbon nanosheets by electrostatic interaction; then, trimesic acid (Hbtc) acted as the complex agent and TEOA as a base for the deprotonation of Hbtc and a template, which leads to in situ growing the MOF on the carbon nanosheets obtaining a sandwich-like structure. Different types of surface analysis techniques were employed to characterize the GO-TEOA@MOFs and g-CN-TEOA@MOFs nanomaterials fabricated. The GO-TEOA@MOFs or g-CN-TEOA@MOFs nanomaterial-modified electrode brings out obviously enhanced electrochemiluminescence (ECL) behaviors due to numerous TEOA in the framework structures. Specifically, both TEOA and GO can serve as the co-reactants for the ECL system of Ru(bpy) and have the synergic effect of enhancing the signal. Based on the GO-TEOA@MOFs modified electrodes, we developed a sensitive and rapid label-free ECL immunoassay strategy for human copeptin, and the linear range was 5 pg mL to 500 ng mL as well as the limit of detection was 360 fg mL. This work exhibits excellent specificity and good stability of the prepared immunosensor in the practical sample determination, demonstrating it can serve as a very promising method for the clinical diagnostics of acute myocardial infarction disease.
一种简便的策略，通过自组装技术将三乙醇胺（TEOA）功能化的金属有机骨架（TEOA@MOF）原位生长在二维氧化石墨烯（GO）或 g-CN 纳米片上。在该方法中，Zn 通过静电相互作用首先附着在碳纳米片上；然后，均苯三甲酸（Hbtc）作为络合剂，TEOA 作为 Hbtc 去质子化和模板的碱，导致 MOF 原位生长在碳纳米片上，获得三明治状结构。采用不同类型的表面分析技术对制备的 GO-TEOA@MOFs 和 g-CN-TEOA@MOFs 纳米材料进行了表征。GO-TEOA@MOFs 或 g-CN-TEOA@MOFs 纳米材料修饰电极由于在骨架结构中存在大量的 TEOA，表现出明显增强的电化学发光（ECL）行为。具体而言，TEOA 和 GO 均可作为 Ru(bpy)的 ECL 体系的共反应物，并具有增强信号的协同效应。基于 GO-TEOA@MOFs 修饰电极，我们开发了一种用于人 copeptin 的灵敏、快速的无标记 ECL 免疫分析策略，线性范围为 5 pg mL 至 500 ng mL，检测限为 360 fg mL。该工作在实际样品测定中表现出所制备的免疫传感器具有优异的特异性和良好的稳定性，表明它可以作为急性心肌梗死疾病临床诊断的一种很有前途的方法。
