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Direct Probing of Organic Peroxy Radical Autoxidation and Cross Reactions

有机过氧自由基自氧化和交叉反应的直接探测

基本信息

批准号：
1807204
负责人：
Joel Thornton
金额：
$ 46.08万
依托单位：
University of Washington
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-08-01 至 2022-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1807204&HistoricalAwards=false
关键词：
Direct Probing Organic Peroxy Radical

项目摘要

This award is supported by the Environmental Chemical Sciences Program of the Division of Chemistry. Professor Joel Thornton of the University of Washington and his group investigate what happens to reactive organic carbon species in the Earth's atmosphere. The highly reactive organic peroxy radicals are common species produced when carbon-based (organic) compounds degrade in the environment. Their detection and quantification is difficult because of their reactivity. Often only a total of organic peroxy radicals are measured, or only early decomposition products are identified. This project involves novel laboratory studies of the reactivity of these species which provides more detailed information than previously possible. An accurate understanding of the fundamental pathways of environmental degradation is crucial to determining what happens to pollutants as they naturally cycle through the Earth's environment. Improved experimental data are necessary for understanding how fuel combustion impacts the atmosphere, aquatic ecosystems, and soil composition. The project provides educational and training opportunities for graduate students, undergraduates in chemistry and atmospheric sciences, and a postdoctoral research fellow. To inform the public of the results of this research, a computer animation is being produced in collaboration with a documentary filmmaker. This film shows how organic peroxy radicals produced in forests contribute to atmospheric particle formation and growth. This research is important to society as it promotes public health and understanding of weather and storms.This project uses fast flow tube reactors coupled to high resolution time of flight and orbitrap mass spectrometers. These techniques allow researchers to identify and simultaneously track nearly all individual organic peroxy radicals and their cross-reaction products. Reaction tracking of a suite of relevant starting compounds, purchased commercially or synthesized by collaborators, is done as a function of reaction time. These experiments provide quantitative insights into the rates and products of gas-phase organic carbon degradation under typical environmental conditions. Isotopic labeling and competitive reactant experiments allow for tests of hypothesized reaction mechanisms and independent rate quantification.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

该奖项由化学部环境化学科学计划支持。华盛顿大学的Joel Thornton教授和他的团队正在研究地球大气中活性有机碳物种的变化。高活性有机过氧自由基是碳基（有机）化合物在环境中降解时产生的常见物质。由于它们的反应性，它们的检测和定量是困难的。通常仅测量有机过氧自由基的总量，或者仅鉴定早期分解产物。该项目涉及对这些物种的反应性进行新的实验室研究，提供了比以前更详细的信息。准确了解环境退化的基本途径对于确定污染物在地球环境中自然循环时发生的情况至关重要。改进的实验数据对于了解燃料燃烧如何影响大气、水生生态系统和土壤成分是必要的。该项目为研究生、化学和大气科学本科生以及一名博士后研究员提供教育和培训机会。为了让公众了解这项研究的结果，正在与一名纪录片制片人合作制作一部电脑动画。这部电影展示了森林中产生的有机过氧自由基如何促进大气颗粒物的形成和增长。这项研究对社会很重要，因为它促进了公众健康和对天气和风暴的了解。该项目使用快速流管反应器，结合高分辨率飞行时间和轨道阱质谱仪。这些技术使研究人员能够识别并同时追踪几乎所有单个有机过氧自由基及其交叉反应产物。一套相关的起始化合物，商业购买或合作者合成的反应跟踪，作为反应时间的函数。这些实验提供了典型环境条件下气相有机碳降解的速率和产物的定量见解。同位素标记和竞争性反应物实验允许测试假设的反应机制和独立的速率量化。该奖项反映了NSF的法定使命，并已被认为是值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持。