Electrochemical Probing through a Redox Capacitor To Acquire Chemical Information on Biothiols.
Electrochemical Probing through a Redox Capacitor To Acquire Chemical Information on Biothiols.
复制标题
通过氧化还原电容器进行电化学探测以获取生物硫醇的化学信息
DOI：
10.1021/acs.analchem.6b01394
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发表时间：
2016-07-19
影响因子：
7.4
通讯作者：
Payne GF
中科院分区：
文献类型：
--
作者：
Liu Z;Liu Y;Kim E;Bentley WE;Payne GF
化学信息的获取对于医学诊断、食品/环境监测以及国家安全至关重要。在此，我们报道了一种电化学信息处理方法，它整合了（i）复杂的电输入/输出，（ii）将电输入/输出转换为能够主动探测化学环境的氧化还原信号的介质，以及（iii）一个用于操纵信号以进行信息提取的氧化还原电容器。由于生物硫醇在医学中的重要性日益凸显，且其独特的化学性质允许对基于假设驱动的信息探测进行评估，我们利用生物硫醇展示了这种化学信息处理策略的能力。我们表明输入序列可以定制，以便从定性（阶跃输入探测硫醇特异性特征）和定量两方面探测化学信息。具体而言，我们观察到了皮摩尔级的检测限以及对超过5个数量级（1皮摩尔 - 0.1微摩尔）浓度的线性响应。这种方法使得信号处理能力得以扩展，可用于化学信息的快速、可靠和现场分析。
The acquisition of chemical information is a critical need for medical diagnostics, food/environmental monitoring, and national security. Here, we report an electrochemical information processing approach that integrates (i) complex electrical inputs/outputs, (ii) mediators to transduce the electrical I/O into redox signals that can actively probe the chemical environment, and (iii) a redox capacitor that manipulates signals for information extraction. We demonstrate the capabilities of this chemical information processing strategy using biothiols because of the emerging importance of these molecules in medicine and because their distinct chemical properties allow evaluation of hypothesis-driven information probing. We show that input sequences can be tailored to probe for chemical information both qualitatively (step inputs probe for thiol-specific signatures) and quantitatively. Specifically, we observed picomolar limits of detection and linear responses to concentrations over 5 orders of magnitude (1 pM–0.1 μM). This approach allows the capabilities of signal processing to be extended for rapid, robust, and on-site analysis of chemical information.