Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, PR China.
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, PR China; Department of Chemistry, Sungkyunkwan University, Suwon, 16419, Republic of Korea.
Biosens Bioelectron. 2024 Dec 15;266:116726. doi: 10.1016/j.bios.2024.116726. Epub 2024 Aug 30.
The oriented design of reticular materials as emitters can significantly enhance the sensitivity of electrochemiluminescence (ECL) sensing analysis for disease markers. However, due to the structural fragility of hydrogen bonds, relational research on hydrogen-bonded organic frameworks (HOFs) has not been thoroughly conducted. Additionally, the modulation of luminescence behavior through HOFs has been rarely reported. In view of this, hydrogen-bonded biohybrid organic frameworks (HBOFs) were synthesized and recruited for ECL immunoassay applications. HBOFs was easily prepared using 6,6',6″,6‴-(pyrene-1,3,6,8-tetrayl)tetrakis(2-naphthoic acid) as linkers via bovine serum albumin (BSA) activated hydrogen-bonded cross-linking. The material exhibited good fluorescence emission characteristics. And the highly ordered topological structure and molecular motion limitation mediated by BSA overcome aggregation-caused quenching and generate strong aggregation induced emission, expressing hydrogen-bond interaction enhanced ECL (HIE-ECL) activity with the participation of tri-n-propylamine. Furthermore, a sandwich immunosensor was constructed employing cobalt-based metal-phenolic network (CMPN) coated ferrocene nanoparticles (FNPs) as quenchers (CMPN@FNPs). Signal closure can be achieved by annihilating the excited state through electron transfer from both CMPN and FNPs. Using a universal disease marker, carcinoembryonic antigen, as the analysis model, the signal-off sensor obtained a detection limit of 0.47 pg/mL within the detection range of 1 pg/mL - 50 ng/mL. The synthesis and application of highly stable HBOFs triggered by proteins provide a reference for the development of new reticular ECL signal labels, and electron transfer model provides flexible solutions for more sensitive sensing analysis.
网状材料的定向设计作为发射器可以显著提高电化学发光（ECL）传感分析对疾病标志物的灵敏度。然而，由于氢键的结构脆弱性，对氢键有机框架（HOFs）的相关研究尚未得到彻底开展。此外，通过 HOFs 调制发光行为的研究也很少有报道。鉴于此，合成了氢键生物杂化有机框架（HBOFs）并将其用于 ECL 免疫分析应用。HBOFs 是通过牛血清白蛋白（BSA）激活氢键交联，使用 6,6',6″,6‴-(芘-1,3,6,8-四羧酸)四(2-萘酸)作为连接体轻松制备的。该材料表现出良好的荧光发射特性。并且 BSA 介导的高度有序拓扑结构和分子运动限制克服了聚集引起的猝灭并产生强烈的聚集诱导发射，表达了氢键相互作用增强的 ECL（HIE-ECL）活性，其中涉及三正丙胺。此外，构建了一种三明治免疫传感器，采用钴基金属-酚网络（CMPN）包覆二茂铁纳米颗粒（FNPs）作为猝灭剂（CMPN@FNPs）。通过 CMPN 和 FNPs 从电子转移中消除激发态，可以实现信号关闭。使用普遍的疾病标志物癌胚抗原作为分析模型，信号关闭传感器在 1 pg/mL - 50 ng/mL 的检测范围内获得了 0.47 pg/mL 的检测限。由蛋白质引发的高度稳定的 HBOFs 的合成和应用为新型网状 ECL 信号标记物的开发提供了参考，电子转移模型为更灵敏的传感分析提供了灵活的解决方案。
