Analytica Chimica Acta ( IF 5.7 ) Pub Date : 2022-02-24 , DOI: 10.1016/j.aca.2022.339648
Yong-Jiang Zhang 1 , Yang Yang 1 , Jun-Mao Wang 1 , Wen-Bin Liang 1 , Ruo Yuan 1 , Dong-Rong Xiao 1
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In this work, a pyrene-based porous organic polymer (Py-POP) with strong electrochemiluminescence (ECL) emission was synthesized and used to fabricate an ECL sensor for the extra-sensitive detection of microRNA-155. The ECL intensity of the Py-POP prepared by tetra(p-aminophenyl)methane (TAPM) and 1,3,6,8-tetrakis(4-formylphenyl)pyrene (TFPPy) was about 3.1 times that of TFPPy aggregates, which was primarily ascribed to the elimination of the effect of aggregation-caused quenching (ACQ) by increasing the distance between ACQ luminophores (pyrene cores) in Py-POP. Meanwhile, the strong covalent connections between 1,3,6,8-tetraphenylpyrene (TPPy) and tetraphenylmethane (TPM) units in the rigid framework of Py-POP could partly block the intramolecular motion of TPPy and TPM, which reduced the non-radiative decay and thus further improved the ECL emission. Furthermore, the hydrophobic porous structure of Py-POP was beneficial to the enrichment of lipophilic tripropylamine (TPrA) coreactants in pores of Py-POP, which greatly shortened the electron migration distance between TPrA coreactants and pyrene luminophores on the pore walls of Py-POP, thereby also enhancing the ECL intensity. By using the Py-POP as a new ECL tag and with the help of the strand displacement processes and target recycling, the fabricated ECL biosensor had a sensitive response for microRNA-155 from 1 fM to 1 nM and a detection limit of 0.326 fM. Overall, this work provided a new and feasible strategy to surmount the ACQ effect for enhancing ECL emission, which not only paved a new way to exploit high-performance ECL materials for fabricating extra-sensitive sensors but also broadened the application of POPs in bioanalysis and ECL fields.
中文翻译:
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通过在芘基多孔有机聚合物中分离 ACQphores 增强电化学发光:一种用于构建生物传感平台的新型 ECL 发射器
在这项工作中,合成了一种具有强电化学发光 (ECL) 发射的芘基多孔有机聚合物 (Py-POP),并用于制造用于超灵敏检测 microRNA-155 的 ECL 传感器。tetra( p ) 制备的 Py-POP 的 ECL 强度-氨基苯基)甲烷(TAPM)和1,3,6,8-四(4-甲酰基苯基)芘(TFPPy)约为TFPPy聚集体的3.1倍,这主要是由于消除了聚集引起的猝灭效应(ACQ) 通过增加 Py-POP 中 ACQ 发光体(芘核)之间的距离。同时,Py-POP刚性框架中1,3,6,8-四苯基芘(TPPy)和四苯基甲烷(TPM)单元之间的强共价连接可以部分阻断TPPy和TPM的分子内运动,从而降低非辐射性。衰减,从而进一步改善 ECL 发射。此外,Py-POP 的疏水多孔结构有利于在 Py-POP 孔隙中富集亲油性三丙胺 (TPrA) 共反应物,这大大缩短了TPrA共反应物与Py-POP孔壁上芘发光体之间的电子迁移距离,从而也增强了ECL强度。通过使用 Py-POP 作为新的 ECL 标签,并在链置换过程和目标回收的帮助下,制造的 ECL 生物传感器对 1 fM 至 1 nM 的 microRNA-155 具有敏感响应,检测限为 0.326 fM。总体而言,这项工作为克服 ACQ 效应以增强 ECL 发射提供了一种新的可行策略,不仅为利用高性能 ECL 材料制造超灵敏传感器开辟了新途径,而且拓宽了 POPs 在生物分析和生物分析中的应用。 ECL 字段。通过使用 Py-POP 作为新的 ECL 标签,并在链置换过程和目标回收的帮助下,制造的 ECL 生物传感器对 1 fM 至 1 nM 的 microRNA-155 具有敏感响应,检测限为 0.326 fM。总体而言,这项工作为克服 ACQ 效应以增强 ECL 发射提供了一种新的可行策略,不仅为利用高性能 ECL 材料制造超灵敏传感器开辟了新途径,而且拓宽了 POPs 在生物分析和生物分析中的应用。 ECL 字段。通过使用 Py-POP 作为新的 ECL 标签,并在链置换过程和目标回收的帮助下,制造的 ECL 生物传感器对 1 fM 至 1 nM 的 microRNA-155 具有敏感响应,检测限为 0.326 fM。总体而言,这项工作为克服 ACQ 效应以增强 ECL 发射提供了一种新的可行策略,不仅为利用高性能 ECL 材料制造超灵敏传感器开辟了新途径,而且拓宽了 POPs 在生物分析和生物分析中的应用。 ECL 字段。