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.

非技术总结本项目支持的研究重点是从根本上了解表面和界面的原子和分子结构和组成之间的联系，以及这些界面的化学性质和反应性。许多重要的技术，从在生产化学品和燃料中使用催化，到电子元件的加工，再到防止腐蚀和结构恶化，都取决于对表面和界面的结构和反应性的了解。本项目包含四个特定的研究课题。第一部分详细探讨了在污染控制和化学生产中重要的催化氧化反应的分子动力学。二是关于结构金属表面氧化和腐蚀的机理及其预防策略。第三部分探讨了表面自组装过程的微观机制，与下一代电子器件的生产以及对生物膜和膜的理解有关。第四个主题寻求开发详细分析复杂表面和界面的方法，这是本研究项目的主题。这些研究课题中的每一个都用于培训学生的研究方法，同时提供支持广泛技术的基础知识。技术总结本研究项目侧重于表面和界面的详细的原子、分子和电子结构与它们的化学性质和反应性之间的联系。这些关于表面结构和反应性的基本问题在四个相互关联的领域中得到了解决。催化氧化的研究主要集中在应用纳米等离子体传感器来评估多相催化氧化反应中催化剂表面中间体的复盖率和存在与否。这些测量获得的机理信息将与半导体激光吸收光谱获得的产品内部状态分布信息相结合，以提供更完整的催化氧化反应动力学图景。第二个领域研究极端环境中的结构合金氧化，以及混合分子缓蚀剂中的协同效应，使用光电子能谱和表面电化学分析。第三个领域涉及有机大分子在液-固界面上的自组装机制，重点是合成基本有趣的化学吸附自组装单分子膜(SAM)，以及定量评估在石墨表面形成物理吸附自组装膜的能量学。第四个领域的工作开发了在X射线光电子能谱中使用静态和动态差异电荷的方法，以便能够对复杂的复合表面材料进行化学和电子性质分析，这是以前研究主题的重点。