Highly Stable Mesoporous Luminescence-Functionalized MOF with Excellent Electrochemiluminescence Property for Ultrasensitive Immunosensor Construction

Abstract

In this work, a novel mesoporous luminescence-functionalized metal-organic framework (Ru-PCN-777) with high stability and excellent electrochemiluminescence (ECL) performance was synthesized by immobilizing Ru(bpy)(mcpbpy) on the Zr cluster of PCN-777 via a strong coordination bond between Zr and -COO. Consequently, the Ru(bpy)(mcpbpy) could not only cover the surface of PCN-777 but also graft into the interior of PCN-777, which greatly increased the loading amount of Ru(bpy)(mcpbpy) and effectively prevented the leaching of the Ru(bpy)(mcpbpy) resulting in a stable and high ECL response. Considering the above merits, we utilized the mesoporous Ru-PCN-777 to construct an ECL immunosensor to detect mucin 1 (MUC1) based on proximity-induced intramolecular DNA strand displacement (PiDSD). The ECL signal was further enhanced by the enzyme-assisted DNA recycling amplification strategy. As expected, the immunosensor had excellent sensitivity, specificity, and responded wide linearly to the concentration of MUC1 from 100 fg/mL to 100 ng/mL with a low detection limit of 33.3 fg/mL (S/N = 3). It is the first time that mesoporous Zr-MOF was introduced into ECL system to assay biomolecules, which might expand the application of mesoporous metal-organic frameworks (MOFs) in bioanalysis. This work indicates that the use of highly stable mesoporous luminescence-functionalized MOFs to enhance the ECL intensity and stability is a feasible strategy for designing and constructing high-performance ECL materials, and therefore may shed light on new ways to develop highly sensitive and selective ECL sensors.

DNA Technology-assisted Signal Amplification Strategies in Electrochemiluminescence Bioanalysis

“…Coupled with efficient metal-organic frameworks (MOF)based ECL emitters of Ru-polyethyleneimine (PEI)@ZIF-8 and AuNPs-PEI@Ru-PCN-777, cyclic amplification process mediated by NEase (Nb.BbvcI) was also adopted for telomerase activity and MUC1 evaluation, respectively [55,56]. Artificial molecular machines can move and function at a single molecular level, attracting considerable attention recently [58,59].…”

Metal-organic Frameworks (MOF)-based Novel Electrochemiluminescence Biosensing Platform for Quantification of H2O2 Releasing from Tumor Cells

“…鉴于其纳米 结构的独特性, MOF 可以作为 ECL 分子的载体, 通过增 大发光体的固载量增强 ECL 响应强度. 如, Hu 等 [19] 合 成了 3D 介孔 MOFs (PCN-777)固载发光体 Ru(bpy) 2 -(mcpbpy [20] , x 0 0…”

Research Progress on Improvement of Conductivity of MOFs and Their Application in Bionsensors: A Review

“…43 The application of 2D MOFs effectively shortens the CT distance, makes CT easier, and improves the efficiency and strength of ECL. According to their experiments, the ECL efficiency of the ECL emitter PEI@Ru-Hf-MOL is 1.27 times higher than the ECL emitter PEI@Ru-PCN-777 (PCN-777 is a 3D MOFs 44 ) and the intensity is 14.5 times higher.…”