Heterogeneous Oxidations of Chemically Diverse Organic Species Relevant to Tropospheric Aerosol Chemistry

与对流层气溶胶化学相关的化学多样性有机物质的非均相氧化

• 批准号: 0856428
• 负责人: Franz Geiger
• 金额: $ 48.2万
• 依托单位: Northwestern University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2009
• 资助国家: 美国
• 起止时间: 2009-07-01 至 2013-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0856428&HistoricalAwards=false
• 关键词: Heterogeneous; Oxidations; Chemically; Diverse; Organic

This award is funded under the American Recovery and Reinvestment Act of 2009 (Public Law 111-5).Understanding the chemistry of organic compounds that are part of atmospheric aerosols is crucial for assessing the impact that aerosols have on climate and the chemical composition of the atmosphere. Given the rich, well documented organic C=C double bond oxidation chemistry, and given the abundance of stereocenters in atmospherically important organic compounds, stereochemistry could play an important role in tropospheric chemical processing, including heterogeneous reactions on aerosol surfaces. However, surprisingly little is known about atmospheric stereochemistry. This project begins to fill this void by applying nonlinear optical spectroscopies, specifically second harmonic generation (SHG) and vibrational sum frequency generation (VSFG) to study the interaction of ozone with surface-active, tropospherically relevant chiral organic compounds, as they yield not only important spectroscopic, structural, and thermodynamic information with surface and molecular specificity, but also the kinetic parameters that are vitally needed for obtaining reliable climate change models. Real-time kinetic measurements, combined with surface spectroscopic studies, allow elucidation of heterogeneous organic oxidation reaction mechanisms.In addition to expanding the fundamental understanding of real-world heterogeneous chemistry in the context of environmental contamination the results of this project also enable advances in existing theoretical and mechanistic frameworks for interfacial phenomena found in nature. This, in turn, advances molecular-level concepts of the fundamental processes governing heterogeneous chemistry in general and helps improve the reliability of predicting the impacts of human activities on the environment. By directly and indirectly interacting with students and policy makers, the integrated research, education, and public outreach activities are powerful tools for communicating the scientific outcomes to the general public.

该奖项是根据2009年美国复苏和再投资法案（公法111-5）资助的。了解作为大气气溶胶组成部分的有机化合物的化学性质，对于评估气溶胶对气候和大气化学成分的影响至关重要。考虑到丰富的有机C=C双键氧化化学，以及在大气中重要的有机化合物中存在丰富的立体中心，立体化学可能在对流层化学过程中发挥重要作用，包括气溶胶表面的非均相反应。然而，令人惊讶的是，我们对大气立体化学知之甚少。该项目开始通过应用非线性光谱学，特别是二次谐波产生（SHG）和振动和频率产生（VSFG）来研究臭氧与表面活性、对流层相关的手性有机化合物的相互作用来填补这一空白，因为它们不仅能产生具有表面和分子特异性的重要光谱、结构和热力学信息，而且动力学参数对于获得可靠的气候变化模型至关重要。实时动力学测量，结合表面光谱研究，允许阐明非均相有机氧化反应机制。除了在环境污染的背景下扩展对现实世界多相化学的基本理解外，该项目的结果还使自然界中发现的界面现象的现有理论和机制框架取得进展。这反过来又推进了分子水平上控制多相化学基本过程的概念，并有助于提高预测人类活动对环境影响的可靠性。通过直接或间接地与学生和政策制定者互动，综合研究、教育和公众宣传活动是向公众传播科学成果的有力工具。