In Situ Optical Detection of Amines at a Parts-per-Quadrillion Level by Severing the Through-Space Conjugated Supramolecular Domino,Journal of the American Chemical Society

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In Situ Optical Detection of Amines at a Parts-per-Quadrillion Level by Severing the Through-Space Conjugated Supramolecular Domino
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-01-17 , DOI: 10.1021/jacs.3c11480
Jiamao Chen _{1,

2} , Yuanyuan Chen _{1,

2} , Jie Liu _{1,

3} , Shiyu Feng _{1,

3} , Wei Huang _{1,

2} , Yao Ling _{1,

3} , Yu Dong _{1,

3} , Weiguo Huang _{1,

3}

Affiliation

Conventional fluorophores suffer from low sensitivity and selectivity in amine detection due to the inherent limitations in their “one-to-one” stoichiometric sensing mechanism. Herein, we propose a “one-to-many” chain reaction-like sensing mechanism by creating a domino chain consisting of one fluorescent molecule (e.g., PTF1) and up to 40 nonemissive polymer chains (pPFPA) comprising over thousand repeating units (PFPA). PTF1 (the domino trigger) interacts with adjacent PFPA units (the following blocks) through polar−π interactions and initiates the domino effect, creating effective through-space conjugation along pPFPA chains and generating amplified yellow fluorescent signals through charge transfer between PTF1 and pPFPA. Amine exposure causes rapid dismantling of the fluorophore-pPFPA-based domino chain and significantly reduces the amplified emissions, thus providing an ultrasensitive method for detecting amines. Relying on the above merits, we achieve a limit of detection of 177 ppq (or 1.67 × 10^–12 M) for triethylamine, which is nearly 4 orders lower than that of previous methods. Additionally, the distinct reactivity of pPFPA toward different amines allows for the discrimination of primary, secondary, and tertiary amines. This study presents a “domino effect” sensing mechanism that has not yet been reported and provides a general approach for chemical detection that is beyond the reach of conventional methods.

中文翻译：

通过切断空间共轭超分子多米诺骨牌，对千万亿分之一的胺进行原位光学检测

传统荧光团由于其“一对一”化学计量传感机制的固有局限性，在胺检测中灵敏度和选择性较低。在此，我们提出了一种“一对多”链式反应式传感机制，通过创建由一个荧光分子（例如 PTF1）和多达 40 个包含数千个重复单元（PFPA）的非发射聚合物链（pPFPA）组成的多米诺骨牌链来实现。）。 PTF1（多米诺触发器）通过极性-π相互作用与相邻的PFPA单元（以下块）相互作用，并引发多米诺骨牌效应，沿着pPFPA链产生有效的空间共轭，并通过PTF1和pPFPA之间的电荷转移产生放大的黄色荧光信号。胺暴露会导致基于荧光团 pPFPA 的多米诺链快速分解，并显着减少放大发射，从而为检测胺提供超灵敏的方法。凭借上述优点，我们实现了三乙胺的检测限为177 ppq（或1.67 × 10 ^–12 M），比之前的方法低了近4个数量级。此外，pPFPA 对不同胺的独特反应性可以区分伯胺、仲胺和叔胺。这项研究提出了一种尚未报道的“多米诺骨牌效应”传感机制，并提供了一种常规方法无法达到的化学检测的通用方法。

更新日期：2024-01-17

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