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

涉及吸附物质的氧化还原反应的原位时间分辨光谱研究

• 批准号: 1412060
• 负责人: Daniel Scherson
• 金额: $ 49.5万
• 依托单位: Case Western Reserve University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2014
• 资助国家: 美国
• 起止时间: 2014-08-15 至 2019-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1412060&HistoricalAwards=false
• 关键词: situ; Time; Resolved; Spectroscopic; Studies

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.

凯斯西储大学的Daniel A. Scherson教授受到化学系化学测量和成像项目的支持，研究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质。重点集中在开发和实施的光谱技术，以监测这些物种在纳秒域的时间演变和控制反应途径的因素。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，例如由过度使用肥料引起的社会问题，以及能源储存和转换。本项目侧重于这些反应的不可逆吸附电催化剂的原位静态和动态表征，以及选择裸和原子修饰的单晶金属表面的微形貌对吸附中间体性质和其他界面性质的影响。这些问题将从微电极耦合、电荷注入和一系列互补的基于显微镜的光谱技术（包括紫外可见反射光谱、共振和表面增强拉曼光谱、和频率和二次谐波产生）中得到深入的了解。这项工作的成功将提供一种将原位光谱电化学技术扩展到纳秒范围的方法，允许研究与各种其他领域相关的电子转移事件的动态方面，包括电催化、多相催化、腐蚀、传感器和环境科学。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。