State Key Laboratory of Electroanalytical Chemistry , Changchun Institute of Applied Chemistry , Changchun , Jilin 130022 , China.
University of Science and Technology of China , Hefei , Anhui 230026 , China.
Anal Chem. 2019 Aug 6;91(15):10156-10163. doi: 10.1021/acs.analchem.9b02169. Epub 2019 Jul 8.
Electrochemiluminescence (ECL)-functionalized metal-organic frameworks (MOFs) have attracted increasing attention in biosensing in virtue of their diverse and tunable optical properties. A famous ECL luminophore, carboxyl-rich tris(4,4'-dicarboxylic acid-2,2'-bipyridyl) ruthenium(II) (Ru(dcbpy)), possesses the characteristics of good water solubility and excellent ECL performance and also has the potential to be the organic ligand of metal-organic frameworks. Herein, functionalized MOF nanosheets (RuMOFNSs) containing plenty of Ru(dcbpy) in the frameworks were synthesized in aqueous solution by a simple one-pot method. In this protocol, Ru(dcbpy) acted as organic ligand to coordinate with Zn originated from Zn(NO), and polyvinylpyrrolidone (PVP) was used as structure-directing agent to control the formation of sheetlike structure. For practical application, a "signal-on" ECL immunosensor was designed for cardiac troponin I (cTnI) detection by employing RuMOFNSs as ECL probe. The immunosensor exhibited high sensitivity and excellent selectivity for cTnI detection in the range from 1 fg/mL to 10 ng/mL with a detection limit as low as 0.48 fg/mL. Finally, the biosensor was successfully applied for the detection of cTnI in human serum sample with satisfactory results, demonstrating its potential application in bioanalysis and clinical diagnosis.
电化学发光（ECL）功能化金属有机骨架（MOFs）由于其多样且可调谐的光学性质，在生物传感中引起了越来越多的关注。一种著名的 ECL 发光体，富羧基三（4,4'-二羧酸-2,2'-联吡啶）钌（II）（Ru(dcbpy)），具有良好的水溶性和出色的 ECL 性能的特点，并且有可能成为金属-有机骨架的有机配体。在此，通过简单的一锅法在水溶液中合成了含有大量 Ru(dcbpy)的功能化 MOF 纳米片（RuMOFNSs）。在该方案中，Ru(dcbpy)作为有机配体与 Zn(NO) 中的 Zn 配位，而聚乙烯吡咯烷酮（PVP）则用作结构导向剂来控制片状结构的形成。为了实际应用，通过将 RuMOFNSs 用作 ECL 探针，设计了用于检测心肌肌钙蛋白 I（cTnI）的“信号开启”ECL 免疫传感器。该免疫传感器在 1 fg/mL 至 10 ng/mL 的范围内对 cTnI 具有高灵敏度和出色的选择性，检测限低至 0.48 fg/mL。最后，该生物传感器成功应用于人血清样本中 cTnI 的检测，结果令人满意，证明了其在生物分析和临床诊断中的潜在应用。
