Collaborative Research: Atmospheric Nanoparticle Growth from Nitrate (NO3) Radical Initiated Oxidation of Monoterpenes

合作研究：硝酸盐 (NO3) 自由基引发的单萜氧化在大气中生长纳米颗粒

• 批准号: 1762098
• 负责人: James Smith
• 金额: $ 45.93万
• 依托单位: University of California-Irvine
• 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: 2018-05-15 至 2022-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1762098&HistoricalAwards=false
• 关键词: Collaborative; Research; Atmospheric; Nanoparticle; Growth

This project combines the results of laboratory studies with numerical modeling to investigate the growth of tiny nanoparticles in the atmosphere. It is important to understand the growth of these tiny particles because they can influence the formation and properties of cloud droplets. This research will lead to the development of a mechanistic model to better predict the influence of aerosol on climate and air quality. Laboratory experiments will be conducted to identify and quantify the gas- and particle-phase products of the reactions of NO3 radicals with three common monoterpenes: α-pinene, β-pinene, 3-carene, and an additional compound, α-thujene, which is structurally similar to α-pinene and should likewise form gas phase products that contribute minimally to nanoparticle growth. These experiments will be conducted for a range of NO3 concentrations, humidities, and temperatures. Computational chemistry studies will provide insight into possible reaction mechanisms and nanoparticle growth due to monoterpene oxidation by NO3 radicals.The three objectives of the project are: (1) Implement computational chemistry methods for elucidating reaction pathways and developing CIMS detection strategies; (2) Perform comparative laboratory studies of NO3 radical initiated oxidation of monoterpenes; and (3) Obtain chemical closure between gas phase precursors and nanoparticle physicochemical properties. The process-level model for nanoparticle growth, developed through this project, will be tested using experimentally measured growth rates. Nanoparticle growth is directly tied to the ability of these particles to influence cloud condensation nuclei populations and affect the formation and properties of cloud droplets. This collaborative project includes a "near-peer" program that pairs University of California at Irvine graduate students with Reed College undergraduates in order to facilitate scientific interactions and to prepare the undergraduates for graduate study.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.

该项目将实验室研究结果与数值模型相结合，研究大气中微小纳米颗粒的生长。了解这些微小颗粒的生长非常重要，因为它们可以影响云滴的形成和特性。这项研究将导致机械模型的开发，以更好地预测气溶胶对气候和空气质量的影响。 将进行实验室实验来识别和量化 NO3 自由基与三种常见单萜反应的气相和颗粒相产物：β-蒎烯、β-蒎烯、3-蒈烯和其他化合物, β-侧柏烯，其结构与 β-蒎烯类似，同样会形成对纳米粒子生长贡献最小的气相产物。这些实验将在一系列 NO3 浓度、湿度和温度下进行。计算化学研究将深入了解单萜被 NO3 自由基氧化导致的可能反应机制和纳米颗粒生长。该项目的三个目标是： (1) 实施计算化学方法来阐明反应途径并开发 CIMS 检测策略； (2) 对NO3自由基引发的单萜氧化进行比较实验室研究； (3)获得气相前体和纳米颗粒物理化学性质之间的化学闭合。通过该项目开发的纳米粒子生长的过程级模型将使用实验测量的生长速率进行测试。纳米粒子的生长与这些粒子影响云凝结核群以及影响云滴的形成和性质的能力直接相关。 该合作项目包括一个“近同行”计划，将加州大学欧文分校的研究生与里德学院的本科生配对，以促进科学互动并为本科生的研究生学习做好准备。该奖项反映了 NSF 的法定使命，并被认为是值得的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来获得支持。

项目成果

Observations of gas-phase products from the nitrate-radical-initiated oxidation of four monoterpenes

四种单萜的硝酸盐自由基引发氧化的气相产物的观察

• DOI: 10.5194/acp-22-9017-2022
• 发表时间: 2022
• 期刊: Atmospheric Chemistry and Physics
• 影响因子: 6.3
• 作者: Dam, Michelia;Draper, Danielle C.;Marsavin, Andrey;Fry, Juliane L.;Smith, James N.
• 通讯作者: Smith, James N.

Chemical Composition of an Ultrafine Sea Spray Aerosol during the Sea Spray Chemistry and Particle Evolution Experiment

• DOI: 10.1021/acsearthspacechem.2c00127
• 发表时间: 2022-07-06
• 期刊: ACS EARTH AND SPACE CHEMISTRY
• 影响因子: 3.4
• 作者: Glicker, Hayley S.;Lawler, Michael J.;Smith, James N.
• 通讯作者: Smith, James N.

Atmospheric clusters to nanoparticles: Recent progress and challenges in closing the gap in chemical composition

• DOI: 10.1016/j.jaerosci.2020.105733
• 发表时间: 2020-12
• 期刊: Journal of Aerosol Science
• 影响因子: 4.5
• 作者: J. Smith;D. Draper;Sabrina Chee;Michelia Dam;Hayley Glicker;Deanna Myers;Adam E. Thomas;M. Lawler;N. Myllys

Relative humidity effect on the formation of highly oxidized molecules and new particles during monoterpene oxidation

• DOI: 10.5194/acp-19-1555-2019
• 发表时间: 2019-02-06
• 期刊: ATMOSPHERIC CHEMISTRY AND PHYSICS
• 影响因子: 6.3
• 作者: Li, Xiaoxiao;Chee, Sabrina;Smith, James N.
• 通讯作者: Smith, James N.