EAGER: Advancing the Analysis of Secondary Organic Aerosols Through Innovations in Soft Ionization Aerosol Mass Spectrometry

EAGER：通过软电离气溶胶质谱的创新推进二次有机气溶胶的分析

• 批准号: 1101194
• 负责人: Giuseppe Petrucci
• 金额: $ 10万
• 依托单位: University of Vermont & State Agricultural College
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-01-01 至 2012-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1101194&HistoricalAwards=false
• 关键词: EAGER; Advancing; Analysis; Secondary; Organic

This project involves developing a more comprehensive understanding of the formation, growth, and aging of biogenic and anthropogenic secondary organic aerosols (BSOA and ASOA, respectively). Atmospheric aerosols play a central role in the atmosphere by influencing global and regional radiative energy balance, visibility, the hydrological cycle, regulation of greenhouse and reactive gases, and human health. SOA is the predominant contributor to submicron atmospheric aerosols, therefore developing an improved understanding of its life cycle in the atmosphere is of great importance. Most chamber-based SOA studies to date have placed emphasis largely on understanding the impact of monoterpenes on the formation and growth of BSOA whilst studies that focus on ASOA typically only employ benzene derivatives with emphasis on toluene, trimethylbenzene, and xylene. There is a need to understand the role of less commonly studied volatile and semivolatile organic compounds (VOC and SVOC, respectively) in SOA formation and atmospheric processing. The goal of this exploratory project is to expand these boundaries to include compounds of basic character (such as amines) which, although potentially important in SOA formation and transformation, have received little attention to date, in large part due to the paucity of suitable analytical methods. The approach will be to develop and utilize an enhanced aerosol mass spectrometry system (i.e., near-infrared laser desorption/ionization AMS, NIR-LDI-AMS) capable of simultaneous measurement of the acidic and basic organic components of SOA, while abnegating extensive fragmentation and rearrangement of ions associated with more vigorous ionization AMS methods. The new, dual-mode instrument will use symmetric reflectron time-of-flight mass spectrometers to measure positive and negative ions from the same aerosol sample. Focus will be placed on the influence of organic nitrogen compounds (ON, such as amines and urea) on the formation, growth and aging of SOA. The studies will include addressing the formation and growth of SOA directly from ON VOCs; and the effects of reactive uptake of ON on SOA, as well as primary organic aerosols (POA). Undergraduate and graduate students will play key roles in implementing and executing experiments in the laboratory as well as disseminating results through presentations and preparation of manuscripts. Students will be trained in several areas, including mass spectrometry, gas/aerosol generation and control, and atmospheric chemistry. The project will also enhance collaborations that have been initiated between the Principal Investigator's group and groups at Harvard University and Amherst College. Results garnered from the studies will be disseminated at national and international conferences, as well as at less formal meetings such as the New England Summer Conference Day on aerosols and atmospheric chemistry, where students and post-doctoral scholars from institutions in the Northeast present results and exchange ideas.

该项目涉及对生物和人为次生有机气溶胶（分别为BSOA和ASOA）的形成、生长和老化进行更全面的了解。大气气溶胶通过影响全球和区域辐射能量平衡、能见度、水文循环、温室气体和反应性气体调节以及人类健康，在大气中发挥核心作用。SOA是亚微米大气气溶胶的主要贡献者，因此发展对其在大气中的生命周期的更好理解是非常重要的。迄今为止，大多数基于腔室的SOA研究主要侧重于理解单萜烯对BSOA形成和生长的影响，而关注ASOA的研究通常只使用苯衍生物，重点是甲苯、三甲苯和二甲苯。有必要了解较少研究的挥发性和半挥发性有机化合物（分别为VOC和SVOC）在SOA形成和大气处理中的作用。这个探索性项目的目标是扩展这些边界，包括基本性质的化合物（如胺），尽管这些化合物在SOA形成和转换中可能很重要，但迄今为止却很少受到关注，这在很大程度上是由于缺乏合适的分析方法。该方法将开发和利用增强型气溶胶质谱系统（即近红外激光解吸/电离AMS， NIR-LDI-AMS），该系统能够同时测量SOA的酸性和碱性有机成分，同时避免与更剧烈的电离AMS方法相关的大量离子碎片和重排。新的双模仪器将使用对称反射飞行时间质谱仪来测量来自同一气溶胶样品的正离子和负离子。重点将放在有机氮化合物（on，如胺和尿素）对SOA形成、生长和老化的影响上。这些研究将包括直接从ON VOCs中解决SOA的形成和发展；以及反应性吸收ON对SOA以及初级有机气溶胶（POA）的影响。本科生和研究生将在实验室实施和执行实验，以及通过报告和准备手稿传播结果方面发挥关键作用。学生将在几个领域接受培训，包括质谱，气体/气溶胶的产生和控制，以及大气化学。该项目还将加强首席研究员小组与哈佛大学和阿默斯特学院小组之间的合作。从这些研究中获得的结果将在国内和国际会议上传播，以及在一些不太正式的会议上传播，比如新英格兰气溶胶和大气化学夏季会议日，在那里，来自东北院校的学生和博士后学者将展示结果并交换意见。