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Dendrimer precursors for nanomolar and picomolar real-time surface plasmon resonance/potentiometric chemical nerve agent sensing using electrochemically crosslinked ultrathin films

机译:使用电化学交联的超薄膜,用于纳摩尔和皮摩尔实时表面等离振子共振/电位化学神经试剂感测的树枝状聚合物前体

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摘要

Nanomolar detection and specific recognition of pinacolyl methylphosphonate (PMP), a hydrolysis product and an analog of a relatively persistent class of toxic nerve agents, has been achieved. In addition, picomolar sensitivity is observed with methylphosphonic acid (MPA), an end-hydrolysis product for all organophosphate-based nerve agents. This is achieved using a combined surface plasmon resonance (SPR) and potentiometry setup. A modified polyamidoamine (PAMAM) carbazole/Cu2+ dendrimer, which is electrochemically crosslinked on a self-assembled monolayer (SAM) modified An substrate, is used as an active sensing element for trapping the nerve-agent analogs. The ultrathin films have been used to study the anchoring of nerve agents via non-covalent interactions. The carbazole to amine ratio is optimized to ensure free primary amines are available to interact with the analyte and the Cu2+ ions present in the system, which further enhances the selectivity. The carbazole group on the periphery serves a dual purpose: crosslinking the dendrimers to form a conjugated network film, and generating the potentiometric response. The adsorption kinetics are monitored by using an in situ SPR/potentiometric setup. This technique not only offers a real-time dual detection of highly toxic nerve-agent analogs, but also shows viability for future sensor-device applications.
机译:已经实现了纳摩尔摩尔检测和精确识别频哪醇甲基膦酸酯(PMP),水解产物和一类相对持久的毒性神经毒剂的类似物。此外,使用甲基膦酸(MPA)观察到皮摩尔敏感性,这是所有基于有机磷酸酯的神经毒剂的最终水解产物。这是通过结合使用表面等离子体激元共振(SPR)和电位计设置来实现的。在自组装单层(SAM)修饰的基质上进行电化学交联的修饰的聚酰胺基胺(PAMAM)咔唑/ Cu2 +树状大分子用作捕获神经制剂类似物的活性传感元件。超薄膜已被用于研究神经药通过非共价相互作用的锚定。咔唑与胺的比例经过优化,以确保游离伯胺可用于与分析物和系统中存在的Cu2 +离子相互作用,从而进一步提高了选择性。外围的咔唑基团具有双重目的:使树枝状聚合物交联以形成共轭网络膜,并产生电位响应。吸附动力学通过使用原位SPR /电位测定装置进行监测。这项技术不仅可以对高毒性神经毒剂类似物进行实时双重检测,而且还显示出了未来传感器设备应用的可行性。

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