Developing Novel Analytical Systems for Deciphering Complex Mixtures of Organic Compounds and Training the Next Generation of Scientists

开发新的分析系统来破译有机化合物的复杂混合物并培训下一代科学家

• 批准号: 1764126
• 负责人: Drew Gentner
• 金额: $ 37.32万
• 依托单位: Yale University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-07-15 至 2023-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1764126&HistoricalAwards=false
• 关键词: Developing; Novel; Analytical; Systems; Deciphering

This project is focused on developing methods for identifying and characterizing specific organic compounds or classes of compounds in a complex mixture of organics in the atmosphere. A large array of sophisticated analytical techniques and instrumentation will be used in the laboratory for optimal characterization of atmospheric gases and aerosols. Understanding the complex composition of gas and particle phase constituents is critically important for air quality studies, especially with regards to determining the toxicity of the inhaled components. The project includes support for graduate and undergraduate students to participate in the research. The project will also involve high school students from the EVOLUTIONS program. The goal of EVOLUTIONS is to supplement the formal school experiences of underserved students to develop transferable skills, STEM literacy, college preparation, and foster aspirations for STEM futures.This proposal involves methods development for offline analytical GC x MS-MS and LC x MS-MS techniques to improve characterization of compound classes that are difficult to measure using online techniques. Laboratory studies will be used to evaluate various analytical configurations for optimal characterization of classes of organics present in atmospheric aerosols, many that are likely important for the characterization of organic aerosol sources and atmospheric processing. In Task 1, an atmospheric pressure chemical ionization (APCI) source and a secondary electrospray ionization (SESI) source will be integrated with an Agilent GC x MS-MS. Method development will be employed to improve thermal extraction of intermediate volatility/ semi-volatile organic carbon (I/SVOCs) collected on adsorbent tubes. Task 2 is focused on LC x MS-MS method development, with specific focus on improving solvent extraction of highly oxygenated molecules (HOM) species collected on adsorbent tubes. Task 3 will intercompare results for target analytes (e.g. I/SVOCs, HOMs, organic nitrates) with an online ToF-CIMS. This work has the potential to contribute new insight to organic aerosol characterization, especially with regards to the intercomparison studies with ToF-CIMS.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.

该项目的重点是开发识别和表征大气中复杂的有机混合物中的特定有机化合物或化合物类别的方法。将在实验室中使用大量复杂的分析技术和仪器，以优化大气气体和气溶胶的特征。了解气体和颗粒相成分的复杂组成对于空气质量研究至关重要，特别是在确定吸入成分的毒性方面。该项目包括为研究生和本科生参与研究提供支持。该项目还将涉及进化计划的高中生。进化论的目标是补充缺乏服务的学生的正规学校经历，以发展可转移的技能、STEM素养、大学准备，并培养对STEM未来的抱负。这项建议涉及离线分析GC x MS和LC x MS-MS技术的方法开发，以改进使用在线技术难以测量的化合物类的表征。将利用实验室研究来评估各种分析配置，以最佳地确定大气气溶胶中存在的有机物类别，其中许多可能对确定有机气溶胶来源和大气加工的特征很重要。在任务1中，大气压化学电离(APCI)源和二次电喷雾电离(SESI)源将与安捷伦GC x MS-MS集成。将利用开发的方法来改进吸附管内收集的中间挥发性/半挥发性有机碳(I/SVOCs)的热提取。任务2的重点是LC x MS-MS方法的开发，特别侧重于改进吸附管内收集的高含氧分子(Hom)的溶剂萃取。任务3将目标分析物(如I/SVOCs、HOMS、有机硝酸盐)的结果与在线TOF-CIMS进行相互比较。这项工作有可能为有机气溶胶的表征贡献新的见解，特别是关于与TOF-CIM的相互比较研究。这一奖项反映了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。

项目成果

Advances in offline approaches for trace measurements of complex organic compound mixtures via soft ionization and high-resolution tandem mass spectrometry

通过软电离和高分辨率串联质谱离线测量复杂有机化合物混合物的进展

• DOI: 10.1016/j.chroma.2019.03.037
• 发表时间: 2019
• 期刊: Journal of Chromatography A
• 影响因子: 4.1
• 作者: Khare, Peeyush;Marcotte, Aurelie;Sheu, Roger;Walsh, Anna N.;Ditto, Jenna C.;Gentner, Drew R.
• 通讯作者: Gentner, Drew R.

Effects of Molecular-Level Compositional Variability in Organic Aerosol on Phase State and Thermodynamic Mixing Behavior

• DOI: 10.1021/acs.est.9b02664
• 发表时间: 2019-11-19
• 期刊: ENVIRONMENTAL SCIENCE & TECHNOLOGY
• 影响因子: 11.4
• 作者: Ditto, Jenna C.;Joo, Taekyu;Gentner, Drew R.
• 通讯作者: Gentner, Drew R.

Analysis of reduced and oxidized nitrogen-containing organic compounds at a coastal site in summer and winter

• DOI: 10.5194/acp-22-3045-2022
• 发表时间: 2022-03-08
• 期刊: ATMOSPHERIC CHEMISTRY AND PHYSICS
• 影响因子: 6.3
• 作者: Ditto, Jenna C.;Machesky, Jo;Gentner, Drew R.
• 通讯作者: Gentner, Drew R.

Asphalt-related emissions are a major missing nontraditional source of secondary organic aerosol precursors

• DOI: 10.1126/sciadv.abb9785
• 发表时间: 2020-09-01
• 期刊: SCIENCE ADVANCES
• 影响因子: 13.6
• 作者: Khare, Peeyush;Machesky, Jo;Gentner, Drew R.
• 通讯作者: Gentner, Drew R.

Atmospheric evolution of emissions from a boreal forest fire: the formation of highly functionalized oxygen-, nitrogen-, and sulfur-containing organic compounds

• DOI: 10.5194/acp-21-255-2021
• 发表时间: 2021-01-14
• 期刊: ATMOSPHERIC CHEMISTRY AND PHYSICS
• 影响因子: 6.3
• 作者: Ditto, Jenna C.;He, Megan;Gentner, Drew R.
• 通讯作者: Gentner, Drew R.