Structure and Dynamics in Heterogeneous Reactions

非均相反应中的结构和动力学

• 批准号: 1506989
• 负责人: Andrew Bocarsly
• 金额: $ 55.5万
• 依托单位: Princeton University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-09-01 至 2018-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1506989&HistoricalAwards=false
• 关键词: Structure; Dynamics; Heterogeneous; Reactions

NON-TECHNICAL SUMMARYThe focus of the research supported in this project is to gain a fundamental understanding of the connection between the atomic and molecular structure and composition of surfaces and interfaces, and the chemical properties and reactivity of these interfaces. A large number of important technologies, ranging from the use of catalysis in the production of chemicals and fuels, to the processing of electronic components, to the prevention of corrosion and structural deterioration, depend on an understanding of the structure and reactivity of surfaces and interfaces. Four particular research topics are contained in this project. The first explores the detailed molecular dynamics of catalytic oxidation reactions important in pollution control and chemical production. The second is concerned with mechanisms of surface oxidation and corrosion of structural metals and strategies for its prevention. The third explores the microscopic mechanism of the process of self-assembly at surfaces, relevant to the production of next generation electronic devices and the understanding of bio-films and membranes. The fourth topic seeks to develop methods for the detailed analysis of the complex surfaces and interfaces that are the subject of this research project. Each of these research topics serves to train students in research methods while providing the fundamental knowledge to support a wide array of technologies. TECHNICAL SUMMARYThis research project focuses on the connection between the detailed atomic, molecular, and electronic structure of surfaces and interfaces, and their chemical properties and reactivity. These fundamental questions of surface structure and reactivity are addressed in four interrelated areas. Studies of catalytic oxidation focus on the implementation of nanoplasmonic sensors to evaluate the coverage and presence of intermediates on the catalyst surface during heterogeneous catalytic oxidation reactions. Mechanistic information obtained from these measurements will be coupled with product internal state distribution information obtained by diode laser absorption spectroscopy, to provide a more complete picture of the catalytic oxidation reaction dynamics. The second area addresses structural alloy oxidation in extreme environments, and synergistic effects in mixed molecular corrosion inhibitors, using photoelectron spectroscopy and electrochemical analysis of the surfaces. The third area concerns the mechanisms of self-assembly of large organic molecules at the liquid-solid interface, with a focus on the synthesis of fundamentally interesting chemisorbed self-assembled monolayers (SAMs), and the quantitative evaluation of the energetics of formation of physisorbed SAMs on graphite. Work in the fourth area develops methods to use both static and dynamic differential charging in X-ray photoelectron spectroscopy to enable the chemical and electronic property analysis of complex composite surface materials that are the focus of the previous research topics.

非技术总结该项目支持的研究重点是对原子和分子结构与表面和界面的组成之间的联系以及这些接口的化学特性和反应性获得基本理解。 从化学和燃料的生产中的使用，到电子成分的加工到预防腐蚀和结构恶化，取决于对表面和界面的结构的理解，许多重要的技术，从化学和燃料的生产，电子成分的加工到预防腐蚀和结构恶化。 该项目包含四个特定的研究主题。 第一个探讨了在污染控制和化学生产中重要的催化氧化反应的详细分子动力学。 第二个与结构金属的表面氧化和预防策略的腐蚀有关。 第三个探讨了表面自组装过程的微观机制，与下一代电子设备的生产以及对生物膜和膜的理解有关。 第四个主题旨在开发方法，以详细分析该研究项目主题的复杂表面和接口。 这些研究主题中的每一个都可以培训学生采用研究方法，同时提供基本知识以支持各种技术。 技术摘要研究项目的重点是表面和界面的详细原子，分子和电子结构及其化学性质和反应性之间的联系。 这些基本的表面结构和反应性问题在四个相互关联的区域解决。 催化氧化的研究集中于实施纳米质传感器，以评估异质催化氧化反应期间催化剂表面中中间体的覆盖范围和存在。 从这些测量结果获得的机械信息将与二极管激光吸收光谱获得的产物内部状态分布信息相结合，以提供更完整的催化氧化反应反应动力学的图像。第二区域在极端环境中介绍了结构合金氧化，并使用光电子光谱和表面的电化学分析在混合分子腐蚀抑制剂中的协同作用。 第三个区域涉及液态固体界面上大的有机分子自组装的机制，重点是综合基本有趣的化学化学化学自我组装单层（SAMS），以及对石墨上物理式sams形成能量的定量评估。 在第四区域的工作开发了在X射线光电子光谱中同时使用静态和动态差分充电的方法，以实现复杂复合表面材料的化学和电子性能分析，这是先前研究主题的重点。