CAREER: Laboratory Studies on the Chemical Characterization of Atmospheric Emission Sources and their Oxidative Evolution using Novel Instrumentation

职业：使用新型仪器对大气排放源的化学特征及其氧化演化进行实验室研究

• 批准号: 1554061
• 负责人: Brent Williams
• 金额: $ 50万
• 依托单位: Washington University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-03-01 至 2022-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1554061&HistoricalAwards=false
• 关键词: CAREER; Laboratory; Studies; Chemical; Characterization

1554061WilliamsPollutants emitted to the atmosphere have a wide array of natural and anthropogenic origins. These pollutants almost immediately undergo oxidative aging processes that transform their molecular composition, ultimately influencing their fate. Vapor and particle pollutants, either emitted directly or formed from atmospheric photochemistry, have detrimental health impacts and can alter the climate. This proposed project will specifically look at organic compounds which comprise a major fraction of air and particulate pollution. To understand the health and climate impacts of specific emission sources, it is necessary to assign these pollutants to their sources of origin. This project will address improved measurement methods and focused laboratory studies to obtain detailed chemical composition of source-specific gases and particles as they undergo oxidative evolution in the atmosphere.The primary goal of this project is to advance the understanding of the sources and transformation of organics emitted to the atmosphere through (1) creation of new in-situ instrumentation for chemical characterization of gases and particles, (2) controlled laboratory studies of the emissions and gas-to-particle formation pathways/potential from simple precursor vapors to realistic complex sources, (3) development of an open-access and searchable mass spectral and source profile database, and (4) integrated education and outreach activities including an academia/industry research experience program for undergraduates and direct research involvement from grade 6-12 students as part of a Peer Mentoring Pipeline Program. The current understanding of the chemicals released from natural and anthropogenic emission sources is limited, and the knowledge of the subsequent chemical transformations of these chemicals that occur while in the atmosphere is even more limited. At the conclusion of this project, metrics will be available for incorporation in model simulations and for field observation interpretation on volatility- and polarity-resolved source-specific chemical composition at the molecular and compound-class level. Additionally, new parameterizations, reaction mechanisms, and gas-to-particle aerosol production yields will be provided for a variety atmospheric oxidants (e.g., OH, O3, NO3) at different concentrations, for a variety of sources (e.g., single gases of differing volatilities and chemical functionality, simple mixtures, complex real sources), with consideration of other atmospheric variables (e.g., NOx and SO2 additions, seed particle types, and humidity levels). New instrumentation will be produced that extends chemical characterization of these emissions across a range of volatilities (from the most volatile gases to the least volatile condensed-phase material), offering new insights on specific atmospheric transformation pathways and fates of these materials. A new academia/industry research experience program in Atmospheric Science and Technology will offer undergraduate students an opportunity to work in both settings, helping to guide their career paths through first-hand experience. This will strengthen academic/industry connections and advance the field. In addition, grade 6-12 students will play a direct role in laboratory studies through the Peer Mentoring Pipeline Program.

1554061威廉斯排放到大气中的污染物有广泛的自然和人为来源。这些污染物几乎立即经历氧化老化过程，改变其分子组成，最终影响其命运。蒸气和颗粒污染物，无论是直接排放还是由大气光化学形成，都对健康产生有害影响，并可能改变气候。这项拟议的项目将专门研究构成空气和颗粒污染主要部分的有机化合物。为了了解特定排放源的健康和气候影响，有必要将这些污染物分配到其来源。该项目将致力于改进测量方法和重点实验室研究，以获得特定来源的气体和颗粒在大气中经历氧化演变时的详细化学成分。该项目的主要目标是通过以下方式促进对排放到大气中的有机物的来源和转化的理解：（1）创建用于气体和颗粒化学特性的新的现场仪器，（2）对从简单的前体蒸汽到实际的复杂来源的排放和气体到颗粒形成途径/潜力进行受控实验室研究，（3）开发一个开放获取和可搜索的质谱和来源概况数据库，以及（4）综合教育和外展活动，包括为本科生提供的学术界/工业界研究经验计划，以及从六年级开始的直接研究参与-12名学生作为同行指导管道计划的一部分。目前对自然和人为排放源释放的化学品的了解有限，对这些化学品在大气中随后发生的化学变化的了解更是有限。在该项目结束时，将提供指标，用于纳入模型模拟，并用于在分子和化合物级别上对挥发性和极性分辨的特定源化学成分进行实地观察解释。此外，将为各种大气氧化剂（例如，OH、O3、NO3）以不同浓度存在，用于各种来源（例如，具有不同挥发性和化学功能性的单一气体、简单混合物、复杂的真实的源），同时考虑其它大气变量（例如，NOx和SO2添加、种子颗粒类型和湿度水平）。将生产新的仪器，将这些排放物的化学特性扩展到一系列挥发性物质（从最挥发的气体到挥发性最低的凝相物质），为这些物质的具体大气转化途径和命运提供新的见解。在大气科学和技术的一个新的学术界/行业研究经验计划将为本科生提供在这两种环境中工作的机会，通过第一手经验帮助指导他们的职业道路。这将加强学术/行业联系并推动该领域的发展。此外，6-12年级的学生将通过同伴指导管道计划在实验室研究中发挥直接作用。

项目成果

Challenges in Predicting the Filtration Performance of a Novel Sewn Mask: Scale-up from Filter Holder to Mannequin Measurements

• DOI: 10.4209/aaqr.200629
• 发表时间: 2021
• 期刊: Aerosol and Air Quality Research
• 影响因子: 4
• 作者: Audrey J Dang;B. Kumfer;J. T. Bertroche;Jane Olson Glidden;Christopher R. Oxford;Udayabhanu M. Jammalamadaka;Mary Ruppert-Stroescu;A. Scott;J. Morris;C. Gan;Jesse Hu;Bradley King;David Dhanraj;Shruti Choudhary;P. Biswas;R. Axelbaum;K. Meacham;Brett Williams

A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

一种快速来源分配技术，应用于热解吸气溶胶气相色谱仪 (TAG) 的环境有机气溶胶测量

• DOI: 10.5194/amt-9-5637-2016
• 发表时间: 2016
• 期刊: Atmospheric Measurement Techniques
• 影响因子: 3.8
• 作者: Zhang, Yaping;Williams, Brent J.;Goldstein, Allen H.;Docherty, Kenneth S.;Jimenez, Jose L.
• 通讯作者: Jimenez, Jose L.

Development and qualification of a VH-TDMA for the study of pure aerosols

• DOI: 10.1080/02786826.2018.1547358
• 发表时间: 2019-01
• 期刊: Aerosol Science and Technology
• 影响因子: 5.2
• 作者: Christopher R. Oxford;Charles M. Rapp;Yang Wang-;Purushottam Kumar;Daniel Watson;J. Portelli;Eric A. Sussman;Steven Dhawan;Jingkun Jiang;B. Williams

Interpretation of Volatility Tandem Differential Mobility Analyzer (V-TDMA) data for accurate vapor pressure and enthalpy measurement: Operational considerations, multiple charging, and introduction to a new analysis program (TAO)

解释挥发性串联微分迁移率分析仪 (V-TDMA) 数据，以实现准确的蒸气压和焓测量：操作注意事项、多次充电以及新分析程序 (TAO) 介绍

• DOI: 10.1080/02786826.2019.1709617
• 发表时间: 2020
• 期刊: Aerosol Science and Technology
• 影响因子: 5.2
• 作者: Oxford, Christopher R.;Dang, Audrey J.;Rapp, Charles M.;Williams, Brent J.
• 通讯作者: Williams, Brent J.