Electrochemiluminescence Enhanced by Restriction of Intramolecular Motions (RIM): Tetraphenylethylene Microcrystals as a Novel Emitter for Mucin 1 Detection
Electrochemiluminescence Enhanced by Restriction of Intramolecular Motions (RIM): Tetraphenylethylene Microcrystals as a Novel Emitter for Mucin 1 Detection
复制标题
通过限制分子内运动 (RIM) 增强电化学发光：四苯乙烯微晶作为粘蛋白 1 检测的新型发射体
DOI：
10.1021/acs.analchem.8b05949
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发表时间：
2019-03-05
影响因子：
7.4
通讯作者：
Yuan, Ruo
中科院分区：
文献类型：
--
作者：
Jiang, Ming-Hui;Li, Sheng-Kai;Yuan, Ruo
基于六方四苯乙烯微晶体（TPE MCs）在水溶液中表现出的极强的电致化学发光现象，在已有报道的聚集诱导电致化学发光（AI-ECL）增强的能量传递机制的基础上，首次提出了一种新的增强策略--限制分子内运动驱动的ECL（RIM-ECL）增强。聚合状态的TPE（TPE MCs）显示出显著增强的ECL，这是由于分子内运动（RIM）的限制。受TPEMCs独特的发光特性的启发，我们将TPEMCs的新型ECL发射体与靶激活的双足DNA步行者结合在一起，制备了一种灵敏的“关-开”ECL生物传感器，用于粘蛋白1（MUC 1）的检测，其线性范围为1 fg/mL ~ 1 ng/mL，检测限为0.29 fg/mL。TPE MCs所展示的RIM增强ECL为探索聚集有机发射体的进一步应用提供了新的篇章。
Apart from the reported energy transfer mechanism of aggregation-induced electrochemiluminescence (AI-ECL) enhancement, a new strategy named restriction of intramolecular motions-driven ECL (RIM-ECL) enhancement is first proposed based on the phenomenon of a very strong electrochemiluminescence observed on the hexagonal tetraphenylethylene microcrystals (TPE MCs) in aqueous solution, Compared to TPE in molecule-isolation state with faint ECL, TPE in aggregate state (TPE MCs) showed a significantly enhanced ECL that was due to the restriction of intramolecular motions (RIM). Inspired by the unique luminescence characteristic of TPE MCs, we integrated the novel ECL emitter of TPE MCs and target-activated bipedal DNA walker together to fabricate a sensitive "off-on" ECL biosensor for Mucin 1 (MUC1) assay, which exhibited desirable linear response for a concentration scope from 1 fg/mL to 1 ng/mL with a low detection limit of 0.29 fg/mL. The RIM enhanced ECL demonstrated by the TPE MCs provides a new chapter in the exploration of aggregated organic emitters for further applications.