基于哑铃板形 AIEgen 的发光 MOF 具有高量子产率作为自增强 ECL 标签：机制洞察和生物传感应用,Small

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基于哑铃板形 AIEgen 的发光 MOF 具有高量子产率作为自增强 ECL 标签：机制洞察和生物传感应用
Small ( IF 13.0 ) Pub Date : 2022-02-13 , DOI: 10.1002/smll.202106567
Jingshuai Li ₁ , Hongying Jia ₁ , Xiang Ren ₁ , Yuyang Li ₁ , Lei Liu ₁ , Ruiqing Feng ₁ , Hongmin Ma ₁ , Qin Wei ₁

Affiliation

众所周知，高性能电化学发光 (ECL) 发射器在提高 ECL 策略的检测灵敏度方面发挥着至关重要的作用。通过聚集诱导发光发光体（AIEgens）、1,1,2,2-四（4-羧基联苯）乙烯（H ₄ TCBPE）与 Zr(IV) 阳离子的结合，形成哑铃板状金属有机骨架（ MOF) 具有高发光效率被合成为 ECL 标签。生成的 MOF 表现出比 H _{4更强的 ECL 活性}TCBPE 单体和聚集体。在此，这种现象被定义为配位触发的电化学发光（CT-ECL）增强效应。此外，几乎匹配的 ECL 和光致发光 (PL) 光谱暗示了带隙发射机制。值得注意的是，作为共反应物的聚乙烯亚胺 (PEI) 与 MOF 共价连接形成 Zr-TCBPE-PEI 的独特自增强 ECL 复合物，其中由于分子内的共反应加速而捕获了强大的 ECL 信号。基于共振能量转移 (RET) 行为，AuPd@SiO ₂复合材料被设计为高效淬火剂。通过这种方式，构建了一种创新且超灵敏的 ECL 传感器，用于通过夹心式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 ^-1。本研究在设计基于 MOF 的自发光 ECL 材料方面取得了一些进展，从而为扩展用于免疫测定的新型 ECL 发射器铺平了新的途径。

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Dumbbell Plate-Shaped AIEgen-Based Luminescent MOF with High Quantum Yield as Self-Enhanced ECL Tags: Mechanism Insights and Biosensing Application

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 (H₄TCBPE) 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 H₄TCBPE 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@SiO₂ 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⁻¹. 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.

更新日期：2022-02-13

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