In-situ study of electrochemical interfaces modified by adsorbed organic molecules; characterizing heterogeneous adsorbate coverage with application to biosensors

吸附有机分子修饰电化学界面的原位研究；

• 批准号: 203356-2011
• 负责人: Bizzotto, Dan
• 金额: $ 4.01万
• 依托单位: University of British Columbia
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2015
• 资助国家: 加拿大
• 起止时间: 2015-01-01 至 2016-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=569935
• 关键词: situ; study; electrochemical; interfaces; modified

In-situ characterization of electrochemical surfaces modified by adsorbed organic molecules is accomplished using a number of different approaches. We have developed a unique method that combines fluorescence microscopy and electrochemistry. This method is proving useful for characterizing the heterogeneity of surface coating, enabling the study of these surfaces with more detail thereby raising some important questions. The creation of advanced biosensors relies on the modification of surfaces to provide a functional interface that can sense the analyte in solution. A number of interesting motifs have been developed that rely upon the orientation of the adsorbed molecules on the sensor surface. These molecules (eg DNA) can include redox active moieties that provide a simple electrochemical signal (current) that can be used for signal transduction. In some cases, the current decreases upon binding, and this has been observed in buffers and complex media. Recent studies of the DNA modified gold surface with our in-situ fluorescence microscopic method has revealed that these surface, created following current literature procedures, are not homogeneous and are, in fact quite heterogeneous. This surprising result has resulted in a number of questions that this research proposal aims to answer. Are these surfaces as presented in simplified cartoons? Does our method highlight these imperfections, something that is hard to determine using the current analytical methods? Can we change the procedures used to make these sensors to eliminate or minimize these undesirable features? In collaboration with two electrochemical research groups in Europe, we will expand the types of molecules that we will assemble onto the electrode surface (aptamers, peptides, DNA). We aim to understand these sensor surfaces and with our unique in-situ characterization tool, determine the characteristics of the system that contribute to these heterogeneous regions, and assess the impact on sensor response. We also intend to use this method to continue our studies into creating a model of a biomembrane supported on an electrode, and to investigate the nature of the forces that govern the movement of molecules that are electrochemically desorbed.

通过多种不同方法，通过吸附有机分子修饰的电化学表面的原位表征。我们开发了一种独特的方法，可以结合荧光显微镜和电化学。事实证明，该方法可用于表征表面涂层的异质性，从而使这些表面的研究更加详细地提出一些重要的问题。 高级生物传感器的创建依赖于表面的修饰来提供一个可以在溶液中感知分析物的功能接口。已经开发了许多有趣的基序，这些基序依赖于传感器表面上吸附的分子的方向。这些分子（例如DNA）可以包括可提供简单的电化学信号（电流）的氧化还原活性部分，可用于信号转导。在某些情况下，结合后电流减少，并且在缓冲液和复杂培养基中观察到了这一点。使用我们的原位荧光显微镜方法对DNA修饰的金表面的最新研究表明，这些表面是按照当前文献程序而创建的，实际上不是均匀的，实际上是非常异构的。这一令人惊讶的结果导致了这项研究建议旨在回答的许多问题。这些表面是否如简化的漫画中所示？我们的方法是否突出了这些缺陷，这是使用当前分析方法难以确定的？我们可以更改用于制作这些传感器以消除或最小化这些不良功能的过程吗？与欧洲的两个电化学研究小组合作，我们将扩大我们将组装到电极表面（Aptamer，肽，DNA）上的分子的类型。我们旨在了解这些传感器表面并使用我们独特的原位表征工具，确定有助于这些异质区域的系统的特征，并评估对传感器响应的影响。我们还打算使用这种方法继续我们的研究来创建一个在电极上支撑的生物膜模型，并研究控制电化学上解剖分子运动的力的性质。