Constraining sources of emerging and increasing concern: Anthropogenic emissions of organic compounds from non-combustion sources and their potential air quality impacts

空气污染造成严重的健康问题，每年在全世界造成800万人死亡。活性有机化学品（ROCs）是构成烟雾的关键前体。在过去，对ROCs排放的研究主要集中在来自汽车和卡车的燃烧源上。然而，非燃烧ROC源，如屋顶和铺路材料，建筑材料，消费品和包装，现在被认为在空气质量中发挥更大的作用。尽管认识到这一点，但关于非燃烧源ROC排放量和化学组成的可靠数据非常有限。这些信息对于了解它们对人类健康和环境的影响至关重要。该项目的目标是通过调查非燃烧源的复杂混合物的ROC排放来满足这一需求。该研究将使用专门设计的反应室进行，使用尖端的分析技术和工具。该项目的成功完成将通过增加我们对影响室外和室内空气质量的污染物排放的理解而造福社会。这个项目对社会的进一步好处是为研究生、本科生和高中实习生提供教育和培训机会。调查员将促进多样性，并通过参与耶鲁大学的K-12外展活动，加强在科学和工程中代表性不足的群体的参与。人们越来越认识到，非燃烧源的排放在空气质量方面发挥着更大的作用。该项目的目标是解决新兴非燃烧源的气相活性有机化合物（ROC）排放及其随后在城市空气中的化学转化方面的知识差距。为了实现这一目标，Aerodyne Research的PI和合作者将专注于已知、未充分研究和未知有机化学品混合物产生的ROC的表征。该团队将使用一套最先进的高分辨率质谱仪和气相/液相色谱仪在发射和反应室中进行实验。该研究将包括“自下而上”的排放实验，以量化铺路和屋顶沥青材料排放的幅度和化学成分，这是ROC的两个最重要的非燃烧来源。这些实验的一个主要重点将是约束不良的排放途径和化合物类。此外，该团队还将在氧化流动反应器中进行实验，以1）确定来自非燃烧源排放的模型和相关前体混合物的氧化产物和二次有机气溶胶产量，以及2）确定这些复杂混合物中存在的关键单一前体。PI将与美国EPA的排放清单和建模专家以及其他利益相关者积极合作，以传播本研究产生的信息和数据。该项目的成功完成，通过对非燃烧源排放的ROC的排放、归宿和大气化学的新见解和基础知识的发展，有可能对空气污染管理产生变革性影响。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Air pollution causes major health problems and is responsible for 8 million deaths annually worldwide. Reactive organic chemicals (ROCs) are the key precursors that make up smog. In the past, research on the emissions of ROCs has focused primarily on combustion sources from cars and trucks. However, non-combustion ROC sources such as roofing and paving materials, building materials, and consumer products and packaging are now understood to play a larger role in air quality. In spite of this recognition, reliable data on the magnitude and chemical makeup of ROC emissions from non-combustion sources is very limited. Such information is critical to understanding their impact on human health and the environment. The goal of this project is to address this need by investigating the emissions of complex mixtures of ROCs from non-combustion sources. The research will be performed using specially designed reaction chambers using cutting-edge analytical techniques and tools. Successful completion of this project will benefit society by increasing our understanding of pollutant emissions that impact both outdoor and indoor air quality. Further benefits to society from this project result from education and training opportunities to graduate students, undergraduate students, and high school interns. The investigator will promote diversity and enhance the involvement of under-represented groups in science and engineering through engagement in Yale's K-12 outreach activities. Emissions from non-combustion sources are increasingly understood to play a larger role in air quality. The goal of this project is to address knowledge gaps on emissions of gas-phase reactive organic compounds (ROCs) from emerging non-combustion sources and their subsequent chemical transformations in urban air. To achieve this goal, the PI and collaborators at Aerodyne Research will focus on the characterization of ROCs generated by mixtures of known, understudied, and unknown organic chemicals. The team will carry out experiments in emission and reaction chambers using a suite of state-of-the-art high-resolution mass spectrometry and gas/liquid chromatography. The research will include “bottom-up” emissions experiments to quantify the magnitude and chemical composition of emissions from paving and roofing asphalt materials, two of the most important non-combustion sources of ROCs. A major focus of these experiments will be on poorly constrained emissions pathways and compound classes. In addition, the team will also conduct experiments in an oxidation flow reactor to 1) determine the oxidation products and secondary organic aerosol yields from model and relevant precursor mixtures emitted from non-combustion sources, and 2) identify key single precursors present in these complex mixtures. The PI will pursue active collaboration with emissions inventory and modeling experts at the U.S. EPA and other stakeholders to disseminate information and data resulting from this study. The successful completion of this project has potential for transformative impact in air pollution management through the development of new insight and fundamental knowledge on the emission, fate, and atmospheric chemistry of ROCs emitted from non-combustion sources.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.