CAREER: Interplay of Particle Phase State and Thermodynamic Mixing in Secondary Organic Aerosol Formation and Partitioning

职业：二次有机气溶胶形成和分配中颗粒相态和热力学混合的相互作用

• 批准号: 1654104
• 负责人: Manabu Shiraiwa
• 金额: $ 68.68万
• 依托单位: University of California-Irvine
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-07-01 至 2023-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1654104&HistoricalAwards=false
• 关键词: CAREER; Interplay; Particle; Phase; State

Forests and anthropogenic activities emit reactive gases that convert to fine particles by complex processes. Current models are unable to predict this secondary particle production and the particle properties limiting our ability to assess impacts on regional air quality and water cycle. This project will develop a detailed first principles model and calibrate it with measurements to predict secondary fine particle production, their properties and their impacts on ice and cloud formation in convective storms. The educational component will develop a web based interactive computational chemistry model to inform and attract students to atmospheric research.The research will harness a master chemical mechanism and a kinetic multi-layer model of gas-particle interactions in aerosols and clouds that explicitly resolves the phase sensitive reactions and mass transport at the particle surface and bulk. This new model will be constrained by laboratory data on size resolved particle phase and chemical composition of secondary organic aerosol (SOA) formation from organic gases. How this formation mechanism transitions and the SOA properties change as we go from isoprene (biogenic) to naphthalene (anthropogenic) organic gases will be investigated to gain molecular level insight. The simulations will be extended to convective regimes of relative humidity, temperatures and updraft velocities that involve ice-nucleation pathways for SOA particles and compared to recent laboratory measurements.

森林和人为活性发出的反应性气体通过复杂的过程转化为细颗粒。当前模型无法预测这种二次粒子的产生，并且粒子的性质限制了我们评估对区域空气质量和水周期影响的能力。该项目将开发一个详细的第一原理模型，并通过测量值对其进行校准，以预测二级细颗粒的产生，其性质及其对对流风暴中冰和云形成的影响。该教育组件将开发基于Web的交互式计算化学模型，以告知学生并吸引学生进行大气研究。该研究将利用一种主要的化学机制和气溶胶和云中气体粒子相互作用的动力学多层模型，这些模型明确解析了相位敏感的反应，并在粒子表面和大量的粒子表面和大量中分解。该新模型将受到实验室数据的限制，这些数据已解决了有机气体的二次有机气溶胶（SOA）形成的化学粒子相和化学成分。当我们从异戊二烯（生物源）转变为萘（人为）有机气体时，这种形成机制如何变化和SOA特性会发生变化，以获得分子水平的见解。与最近的实验室测量相比，这些模拟将扩展到相对湿度，温度和上升速度的相对湿度，温度和上升速度的对流方案。

项目成果

Timescales of secondary organic aerosols to reach equilibrium at various temperatures and relative humidities

• DOI: 10.5194/acp-19-5959-2019
• 发表时间: 2019-02
• 期刊: Atmospheric Chemistry and Physics
• 影响因子: 6.3
• 作者: Ying Li;M. Shiraiwa

Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene

• DOI: 10.5194/acp-18-1643-2018
• 发表时间: 2018-02-06
• 期刊: ATMOSPHERIC CHEMISTRY AND PHYSICS
• 影响因子: 6.3
• 作者: Hinks, Mallory L.;Montoya-Aguilera, Julia;Nizkorodov, Sergey A.
• 通讯作者: Nizkorodov, Sergey A.

Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors

• DOI: 10.5194/acp-19-12515-2019
• 发表时间: 2019-04
• 期刊: Atmospheric Chemistry and Physics
• 影响因子: 6.3
• 作者: M. Song;Adrian M. Maclean;Yuanzhou Huang;Natalie R. Smith;Sandra L. Blair;J. Laskin;A. Laskin;W. W. Derieux-W.;Ying Li;M. Shiraiwa;S. Nizkorodov;A. Bertram

Influence of particle viscosity on mass transfer and heterogeneous ozonolysis kinetics in aqueous-sucrose-maleic acid aerosol.

• DOI: 10.1039/c8cp01666f
• 发表时间: 2018-06
• 期刊: Physical chemistry chemical physics : PCCP
• 作者: Frances H. Marshall;T. Berkemeier;M. Shiraiwa;L. Nandy;Peter B. Ohm;C. Dutcher;J. Reid

Predicting glass transition temperature and melting point of organic compounds via machine learning and molecular embeddings

• DOI: 10.1039/d1ea00090j
• 发表时间: 2022-05-01
• 期刊: ENVIRONMENTAL SCIENCE-ATMOSPHERES
• 作者: Galeazzo, Tommaso;Shiraiwa, Manabu
• 通讯作者: Shiraiwa, Manabu