Li Jingshuai, Jia Hongying, Ren Xiang, Li Yuyang, Liu Lei, Feng Ruiqing, Ma Hongmin, Wei Qin
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, Shandong, 250022, China.
Small. 2022 Apr;18(13):e2106567. doi: 10.1002/smll.202106567. Epub 2022 Feb 13.
It is widely known that high-performance electrochemiluminescence (ECL) emitters play a crucial part in improving the detection sensitivity of the ECL strategy. Through the combination of aggregation-induced emission luminogens (AIEgens), 1,1,2,2-tetra(4-carboxylbiphenyl)ethylene (H TCBPE) with Zr(IV) cations, a dumbbell plate-shaped metal-organic framework (MOF) with high luminous efficiency is synthesized as ECL tags. The resultant MOF exhibits stronger ECL activity than those of H TCBPE monomers and aggregates. Herein, this phenomenon is defined as the coordination-triggered electrochemiluminescence (CT-ECL) enhancement effect. Furthermore, the nearly matched ECL and photoluminescence (PL) spectra imply the bandgap emission mechanism. Remarkably, polyethyleneimine (PEI) as the coreactant is covalently connected with MOF to form the uniquely self-enhanced ECL complex of Zr-TCBPE-PEI, where the robust ECL signal is captured owing to the intramolecular-like coreaction acceleration. Based on the resonance energy transfer (RET) behavior, the AuPd@SiO composite is designed as the high-efficiency quencher. In this manner, an innovative and ultrasensitive ECL sensor is constructed for neuron-specific enolase (NSE) detection through sandwich-type immunoreaction, with the detection limit down to 52 fg ml . The present study has gone some way toward designing MOF-based self-luminescent ECL materials, thus paving a new avenue to expand the late-model ECL emitters for immunoassay.
众所周知，高性能电化学发光（ECL）发光体在提高ECL策略的检测灵敏度方面起着至关重要的作用。通过将聚集诱导发光剂（AIEgens）1,1,2,2-四（4-羧基联苯）乙烯（H TCBPE）与Zr(IV)阳离子相结合，合成了一种具有高发光效率的哑铃板状金属有机框架（MOF）作为ECL标签。所得的MOF表现出比H TCBPE单体和聚集体更强的ECL活性。在此，这种现象被定义为配位触发电化学发光（CT-ECL）增强效应。此外，近乎匹配的ECL和光致发光（PL）光谱暗示了带隙发射机制。值得注意的是，聚乙烯亚胺（PEI）作为共反应剂与MOF共价连接，形成独特的自增强ECL复合物Zr-TCBPE-PEI，由于分子内样共反应加速，捕获了强大的ECL信号。基于共振能量转移（RET）行为，将AuPd@SiO复合材料设计为高效猝灭剂。通过这种方式，构建了一种创新的超灵敏ECL传感器，用于通过夹心型免疫反应检测神经元特异性烯醇化酶（NSE），检测限低至52 fg/ml。本研究在设计基于MOF的自发光ECL材料方面取得了一定进展，从而为扩展用于免疫分析的新型ECL发光体开辟了一条新途径。
