In situ Time-Resolved Spectroscopic Studies of Redox Reactions Involving Adsorbed Species

丹尼尔教授A.凯斯西储大学的Scherson得到化学系化学测量和成像项目的支持，研究涉及水溶液中分子和离子形式的氮和硫氧化物的反应机制，以及与能量转换和电合成相关的其他物种。重点是集中在光谱技术的发展和实施，用于监测在纳秒域和控制反应途径的因素，这些物种的时间演变原位。这些研究的结果将为解决与环境控制和补救有关的社会问题开辟新的前景，例如过度使用化肥以及能源储存和转换所产生的问题。 该项目的重点是在原位静态和动态特性的不可逆吸附的电催化剂这些反应，以及选定的裸露和原子改性的单晶金属表面上的吸附中间体和其他界面性质的性质的微观形貌的影响。深入了解这些问题将获得从耦合的微电极，电荷注入，和阵列的互补显微镜为基础的光谱技术，包括紫外可见反射光谱，共振和表面增强拉曼光谱，和和频率和二次谐波产生。这项工作的成功将提供一种手段，用于扩展到纳秒范围内的原位光谱电化学技术，允许相关的各种其他领域，包括电催化，多相催化，腐蚀，传感器和环境科学的电子转移事件的动态方面的研究。参与这项研究的学生将接受广泛的基础和应用学科的培训。

Professor Daniel A. Scherson of Case Western Reserve University is supported by the Chemical Measurement and Imaging program of the Division of Chemistry to investigate the mechanism of reactions involving nitrogen and sulfur oxides both in molecular and ionic forms in aqueous solutions, as well as other species of relevance to energy conversion and electrosynthesis. Emphasis is centered on the development and implementation of spectroscopic techniques for monitoring in situ the time evolution of such species in the nanosecond domain and the factors that control the reaction pathways. The results emerging from these studies will open new prospects for addressing societal problems associated with environmental control and remediation, such as those derived from the overuse of fertilizers, and energy storage and conversion. This project focuses on the in situ static and dynamic characterization of irreversibly adsorbed electrocatalysts for these reactions, as well as the effect of the microtopography of selected bare and atom-modified single crystal metal surfaces on the nature of adsorbed intermediates and other interfacial properties. Insight into these issues will be gained from the coupling of microelectrodes, charge injection, and an array of complementary microscope-based spectroscopic techniques, including UV visible reflection spectroscopy, resonance and surface enhanced Raman spectroscopies, and sum frequency and second harmonic generation. The success of this work would provide a means for extending in situ spectroelectrochemical techniques into the nanosecond range, allowing the study of the dynamic aspects of electron transfer events of relevance to a variety of other fields, including electrocatalysis, heterogeneous catalysis, corrosion, sensors, and environmental science. Students involved in this research will be trained in a broad range of fundamental and applied disciplines.