Hydrodynamic Electrochemistry: Investigation of Interfacial Redox Reactions in Materials, Small Molecules, and Biomolecules

如果没有界面电子转移（ET）反应，生命就不会存在。更重要的是，如果我们不能更多地了解这种ET反应，我们所知道的生命可能会不复存在。首先，在每个活细胞中实现功能的生物机制依赖于蛋白质之间、蛋白质与底物之间以及跨细胞膜的界面ET。其次，新兴的可持续、太阳能和分析技术也需要不同的界面ET反应，最重要的是在固体和分析物（水性和非水性）之间的界面。这一建议要求新的电化学设备的研究ET反应的材料，小分子和生物分子。这些设备将用于支持无机、材料、生物和分析化学方面的研究和培训。 具体而言，我们要求一个bipotentiostat和旋转环盘电化学（RRDE）装置。该设备将使我们能够研究上述化学体系的催化电化学行为（在“盘”处），同时探测反应产物的形成和行为（在“环”处）。需要双恒电位仪，因为该实验实际上是同时进行的两个电化学实验。电极旋转器允许对催化动力学和扩散对反应物和产物的影响进行仔细和定量分析。所要求的恒电位仪在实验多样性和仪器灵敏度方面是最先进的。因此，它也将在传统的电化学实验中得到常规使用，包括循环伏安法，脉冲伏安法，光谱电化学和阻抗测量。我们目前无法访问SFU的RRDE系统，因此在没有进一步支持的情况下无法进行拟议的研究。 SFU的化学系拥有广泛的氧化还原反应专业知识。PI（Warren）是蛋白质和小分子氧化还原化学领域的新兴领导者，特别是在对可持续化学至关重要的反应方面（例如，CO2和O2减少）。所需仪器的高灵敏度也是研究蛋白质嵌入辅因子的氧化还原反应的理想选择。其他用户将包括教授。丹尼尔Leznoff和蒂姆Storr，谁有新兴的兴趣在分子材料的发展和研究他们的氧化还原化学。Hogan Yu教授是分析化学方面的专家，他很高兴能够使用我们的新RRDE开发基于DNA酶的新化学传感器。最后，拜伦·盖茨教授在分析化学和可再生燃料/催化研究方面有一个长期的计划。他的团队很高兴使用所要求的设备来研究葡萄糖传感和水氧化的材料。

Life would not exist without interfacial electron transfer (ET) reactions. More importantly, if we fail to learn more about such ET reactions, life as we know it will probably cease to exist. First, the biological machinery that enables function in every living cell relies on interfacial ET between proteins, between proteins and substrates, and across cell membranes. Second, emerging sustainable, solar, and analytical technologies also require diverse interfacial ET reactions, most importantly at interfaces between solids and analytes (both aqueous and non-aqueous). This proposal requests new electrochemical equipment for investigation of ET reactions in materials, small molecules, and biological molecules. Equipment will support research and training in inorganic, materials, biological and analytical chemistries. Specifically, we request a bipotentiostat and rotating ring-disk electrochemistry (RRDE) apparatus. This equipment will allow us to investigate the catalytic electrochemical behaviour of the above chemical systems (at the "disk") while simultaneously probing formation and behaviour of reaction products (at the "ring"). A bipotentiostat is required because this experiment is effectively two electrochemistry experiments at the same time. The electrode rotator allows for careful and quantitative analysis of catalytic kinetics and the effect of diffusion on reaction reactant and products. The requested potentiostat is state-of-the-art in terms of experimental diversity and instrumental sensitivity. As such, it will see routine use in traditional electrochemistry experiments as well, including cyclic voltammetry, pulse voltammetry, spectroelectrochemistry, and impedance measurements. We do not currently have access to an RRDE system at SFU and consequently are unable to carry out the proposed research without further support. The Department of Chemistry at SFU is home to a breadth of expertise in redox reactions. The PI (Warren) is an emerging leader in redox chemistry of proteins and small molecules, especially with respect to reactions important for sustainable chemistry (e.g., CO2 and O2 reduction). The high sensitivity of the requested instrument also is ideal for investigating redox reactions of protein-embedded cofactors. Other users will include Profs. Daniel Leznoff and Tim Storr, who have emerging interests in the development of molecular materials and investigation of their redox chemistries. Prof. Hogan Yu is an expert in analytical chemistry and is excited to use our new RRDE to develop new chemical sensors based on DNAzymes. Finally, Prof. Byron Gates has a longstanding program in analytical chemistry and renewable fuel/catalysis research. His group is excited to use the requested equipment to investigate materials for glucose sensing and water oxidation.