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

新兴和日益关注的限制来源：非燃烧源有机化合物的人为排放及其潜在的空气质量影响

• 批准号: 2011362
• 负责人: Drew Gentner
• 金额: $ 33万
• 依托单位: Yale University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-07-15 至 2024-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2011362&HistoricalAwards=false
• 关键词: Constraining; sources; emerging; increasing; concern

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.

空气污染会导致严重的健康问题，每年导致全球 800 万人死亡。反应性有机化学品 (ROC) 是构成烟雾的关键前体。过去，对 ROC 排放的研究主要集中在汽车和卡车的燃烧源上。然而，现在人们知道，屋顶和铺路材料、建筑材料、消费品和包装等非燃烧 ROC 来源在空气质量方面发挥着更大的作用。尽管认识到这一点，关于非燃烧源 ROC 排放量和化学成分的可靠数据仍然非常有限。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 ROC 混合物的排放来满足这一需求。该研究将使用专门设计的反应室以及尖端的分析技术和工具进行。该项目的成功完成将增加我们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。该项目为研究生、本科生和高中实习生提供的教育和培训机会为社会带来了进一步的好处。研究人员将通过参与耶鲁大学的 K-12 外展活动，促进多样性并加强代表性不足的群体对科学和工程的参与。人们越来越认识到非燃烧源的排放对空气质量起着更大的作用。该项目的目标是解决新兴非燃烧源气相活性有机化合物（ROC）排放及其随后在城市空气中化学转化的知识差距。为了实现这一目标，首席研究员和 Aerodyne Research 的合作者将重点研究已知、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和气/液色谱在发射室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（两种最重要的非燃烧 ROC 来源）的排放量和化学成分。这些实验的主要焦点将是约束不充分的排放途径和化合物类别。此外，该团队还将在氧化流反应器中进行实验，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，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，传播本研究产生的信息和数据。该项目的成功完成，通过发展关于非燃烧源排放的 ROC 的排放、归宿和大气化学的新见解和基础知识，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智力优点和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Anthropogenic secondary organic aerosol and ozone production from asphalt-related emissions

沥青相关排放物产生的人为二次有机气溶胶和臭氧

• DOI: 10.1039/d3ea00066d
• 发表时间: 2023
• 期刊: Environmental Science: Atmospheres
• 作者: Seltzer, Karl M.;Rao, Venkatesh;Pye, Havala O.;Murphy, Benjamin N.;Place, Bryan K.;Khare, Peeyush;Gentner, Drew R.;Allen, Christine;Cooley, David;Mason, Rich
• 通讯作者: Mason, Rich

Real-world observations of reduced nitrogen and ultrafine particles in commercial cooking organic aerosol emissions

• DOI: 10.5194/acp-24-1281-2024
• 发表时间: 2024-01
• 期刊: Atmospheric Chemistry and Physics
• 影响因子: 6.3
• 作者: Sunhye Kim;J. Machesky;D. Gentner;A. Presto

Total organic carbon measurements reveal major gaps in petrochemical emissions reporting

总有机碳测量揭示石化排放报告中的主要差距

• DOI: 10.1126/science.adj6233
• 发表时间: 2024
• 期刊: Science
• 影响因子: 56.9
• 作者: He, Megan;Ditto, Jenna C.;Gardner, Lexie;Machesky, Jo;Hass-Mitchell, Tori N.;Chen, Christina;Khare, Peeyush;Sahin, Bugra;Fortner, John D.;Plata, Desiree L.
• 通讯作者: Plata, Desiree L.

Emerging investigator series: deposited particles and human lung lining fluid are dynamic, chemically-complex reservoirs leading to thirdhand smoke emissions and exposure

新兴研究者系列：沉积颗粒和人体肺内壁液体是动态的、化学复杂的储存库，导致三手烟排放和暴露

• DOI: 10.1039/d1ea00107h
• 发表时间: 2022
• 期刊: Environmental Science: Atmospheres
• 作者: Sheu, Roger;Hass-Mitchell, Tori;Ringsdorf, Akima;Berkemeier, Thomas;Machesky, Jo;Edtbauer, Achim;Klüpfel, Thomas;Filippi, Alexander;Musa Bandowe, Benjamin A.;Wietzoreck, Marco
• 通讯作者: Wietzoreck, Marco