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

空气污染造成了重大的健康问题，每年导致全球800万人死亡。活性有机化学品(ROCs)是构成烟雾的关键前体。过去，对ROC排放的研究主要集中在轿车和卡车的燃烧源上。然而，非燃烧的ROC来源，如屋顶和铺路材料，建筑材料，以及消费品和包装，现在被认为在空气质量中发挥着更大的作用。尽管承认了这一点，但关于非燃烧来源的ROC排放的大小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来自非燃烧来源的复杂的ROCs混合物的排放来满足这一需要。这项研究将使用专门设计的反应室，使用尖端的分析技术和工具。这个项目的成功完成将使我们加深对影响室外和室内空气质量的污染物排放的了解，从而造福社会。通过为研究生、本科生和高中实习生提供教育和培训机会，该项目还将为社会带来更多好处。这位调查员将通过参与耶鲁大学的K-12外联活动，促进多样性，并加强未被充分代表的群体在科学和工程领域的参与。人们越来越多地认识到，非燃烧来源的排放在空气质量中发挥着更大的作用。该项目的目标是解决关于新出现的非燃烧来源的气相活性有机化合物(ROCs)的排放及其随后在城市空气中的化学转化的知识差距。为了实现这一目标，PI和Aerodyne Research的合作者将重点研究已知、未被研究和未知的有机化学品混合物产生的ROC的特征。该团队将使用一套最先进的高分辨率质谱仪和气/液色谱在发射室和反应室进行实验。这项研究将包括“自下而上”的排放实验，以量化路面和屋顶沥青材料排放的数量和化学成分，这两种材料是ROC最重要的非燃烧来源。这些实验的一个主要焦点将是不受限制的排放途径和化合物类别。此外，该小组还将在氧化流动反应器中进行实验，以1)确定模型和非燃烧源排放的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将与美国环保局的排放清单和建模专家以及其他利益攸关方积极合作，传播这项研究产生的信息和数据。该项目的成功完成对空气污染管理具有潜在的变革影响，通过发展对非燃烧来源排放的ROC的排放、命运和大气化学的新见解和基础知识。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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.