Chiral Sensing Using a Complementary Metal-Oxide Semiconductor-Integrated Three-Transducer Microsensor System

Chiral Sensing Using a Complementary Metal-Oxide Semiconductor-Integrated Three-Transducer Microsensor System
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DOI:
10.1021/ac9017007
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发表时间:
2009-11-15
影响因子:
7.4
通讯作者:
Hierlemann, Andreas
Hierlemann, Andreas
中科院分区:
化学1区
文献类型:
--
作者:
Kurzawski, Petra;Schurig, Volker;Hierlemann, Andreas

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将不同的手性环糊精衍生物溶解在聚硅氧烷基质中,并已用作三传感器微系统(包括量热传感器、质量敏感传感器和电容化学传感器)上的敏感涂层。当接触手性分析物(例如乳酸甲酯和 2-氯丙酸甲酯)时,所有三种传感器都对这些分析物表现出明显的手性辨别力。发现这些信号构成了吸附热力学和的卷积。传感器特定的贡献,其中包括,在电容式传感器的情况下,分子取向效应,甚至导致两种对映体产生相反符号的信号。所有三个传感器的传感器响应曲线都可以通过应用一个模型来解释和拟合,该模型本质上意味着代表特定相互作用的朗缪尔等温线(在低浓度下占主导地位)和用于非特异性物理吸附的亨利等温线的叠加。这里公开的结果表明,一方面,传感器技术可用于揭示对映选择性分析物-受体或分析物-基质相互作用的细节,另一方面,由于换能器特定信号贡献,传感器可以提供相对于吸附热力学确定的气相色谱甚至更明显的手性辨别(“辨别增强”)。
Different chiral cyclodextrin derivatives were dissolved in a polysiloxane matrix and have been used as sensitive coatings on a three-transducer microsystem including a calorimetric, a mass-sensitive, and a capacitive chemical sensor. Upon exposure to chiral analytes, such as methyl lactate and methyl-2-chloropropionate, all three transducers showed distinct chiral discrimination of these analytes. The signals were found to constitute a convolution of sorption thermodynamics and. transducer-specific contributions, which included, in the case of the capacitive sensor, molecular orientation effects so that even opposite-sign signals for the two enantiomers resulted. The sensor response curves of all three transducers could be explained and fitted by applying a model that essentially implies the superposition of a Langmuir isotherm representing specific interactions, predominant at low concentrations, and a Henry isotherm for nonspecific physisorption. The results disclosed here show that, on the one hand, sensor techniques can be used to reveal details of enantioselective analyte-receptor or analyte-matrix interactions and that, on the other hand, sensors may provide an even more pronounced chiral discrimination ("discrimination enhancement") with respect to sorption-thermodynamics-determined gas chromatography as a consequence of the transducer-specific signal contributions.