Collaborative Research: Organosulfate Multiphase Chemistry and Physicochemcal Properties--Oxidation and Sulfate Recycling in Aerosols and Cloud Droplets

合作研究：有机硫酸盐多相化学和物理化学性质——气溶胶和云滴中的氧化和硫酸盐回收

• 批准号: 2039788
• 负责人: Jason Surratt
• 金额: $ 47.44万
• 依托单位: University of North Carolina at Chapel Hill
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-03-01 至 2025-02-28
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2039788&HistoricalAwards=false
• 关键词: Collaborative; Research; Organosulfate; Multiphase; Chemistry

This project addresses a gap in the understanding of mechanistic pathways that lead to the formation of particulate organosulfates in the atmosphere. Laboratory studies will be conducted to examine the fate of gaseous isoprene epoxydiols and to study how the products of these reactions might alter the properties of atmospheric aerosol. The results of these studies will help to improve predictions of the formation of secondary organic aerosol in both air quality and climate models.The objectives of this project include the study of: (1) heterogeneous hydroxyl radical (OH) oxidation of isoprene epoxydiol- (IEPOX) derived low-volatility particulate organosulfates (OSs) to understand how relative humidity (RH), pre-existing aerosol composition (including pH), and OH exposure alter daytime OS composition and physicochemical properties; (2) heterogeneous nitrate (NO3) oxidation of IEPOX-derived OSs to understand how RH, pre-existing aerosol composition (including pH), and NO3 exposure alter nighttime OS composition and physicochemical properties; and (3) cloudwater oxidation experiments to understand how particulate IEPOX-derived OSs recycle inorganic sulfate to yield multifunctional OSs, and thus aqueous secondary organic aerosol (SOA) upon cloud droplet evaporation.This project includes outreach efforts to high school students through the NSF-funded Youth Engaging in the Science of Resilience Program and the NIH-funded 21st Century Environmental Health Scholars Program at the University of North Carolina and through the Detroit Research Internship and Summer Experience (D- RISE) program at the University of Michigan.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.

该项目解决了在理解导致大气中颗粒有机硫酸盐形成的机械途径方面的差距。 将进行实验室研究，以检查气体异戊二烯环氧二醇的命运，并研究这些反应的产物如何改变大气气溶胶的性质。 这些研究的结果将有助于改进在空气质量和气候模式中对二次有机气溶胶形成的预测。（1）异戊二烯环氧二醇-（IEPOX）衍生的低挥发性颗粒有机硫酸盐（OS）的非均相羟基自由基（OH）氧化，以了解相对湿度（RH）、预先存在的气溶胶组合物（包括pH值）和OH暴露改变白天OS组成和物理化学性质;（2）IEPOX衍生OS的非均质硝酸盐（NO3）氧化，以了解RH，预先存在的气溶胶组成（包括pH）和NO3暴露改变夜间OS组成和理化性质;和（3）云水氧化实验以了解颗粒状IEPOX衍生的OS如何再循环无机硫酸盐以产生多功能OS，因此，含水二次有机气溶胶（SOA）云滴蒸发。该项目包括通过NSF向高中学生推广工作，在北卡罗来纳州大学资助的青年参与弹性科学计划和NIH资助的21世纪世纪环境卫生学者计划，并通过底特律研究实习和夏季经验（D- RISE）该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的学术价值和更广泛的影响审查标准。

项目成果

Acidity-Dependent Atmospheric Organosulfate Structures and Spectra: Exploration of Protonation State Effects via Raman and Infrared Spectroscopies Combined with Density Functional Theory

酸度依赖的大气有机硫酸盐结构和光谱：通过拉曼和红外光谱结合密度泛函理论探索质子化态效应

• DOI: 10.1021/acs.jpca.2c04548
• 发表时间: 2022
• 期刊: The Journal of Physical Chemistry A
• 作者: Fankhauser, Alison M.;Lei, Ziying;Daley, Kimberly R.;Xiao, Yao;Zhang, Zhenfa;Gold, Avram;Ault, Bruce S.;Surratt, Jason D.;Ault, Andrew P.
• 通讯作者: Ault, Andrew P.

Organosulfate Formation in Proxies for Aged Sea Spray Aerosol: Reactive Uptake of Isoprene Epoxydiols to Acidic Sodium Sulfate

• DOI: 10.1021/acsearthspacechem.2c00156
• 发表时间: 2022-11
• 期刊: ACS Earth and Space Chemistry
• 影响因子: 3.4
• 作者: Madeline E. Cooke;N. C. Armstrong;Ziying Lei;Yuzhi Chen;Cara M. Waters;Yue Zhang-;Nicolas A. Buchenau;Monica Q. Dibley;Isabel R Ledsky;Tessa Szalkowski;Jamy Y. Lee;K. Baumann;Zhenfa Zhang;W. Vizuete;A. Gold;J. Surratt;A. Ault

Heterogeneous Oxidation Products of Fine Particulate Isoprene Epoxydiol-Derived Methyltetrol Sulfates Increase Oxidative Stress and Inflammatory Gene Responses in Human Lung Cells

• DOI: 10.1021/acs.chemrestox.3c00278
• 发表时间: 2023-10-31
• 期刊: CHEMICAL RESEARCH IN TOXICOLOGY
• 影响因子: 4.1
• 作者: Khan，Faria;Chen，Yuzhi;Surratt，Jason D.
• 通讯作者: Surratt，Jason D.

Morphology and Viscosity Changes after Reactive Uptake of Isoprene Epoxydiols in Submicrometer Phase Separated Particles with Secondary Organic Aerosol Formed from Different Volatile Organic Compounds

• DOI: 10.1021/acsearthspacechem.1c00156
• 发表时间: 2022-03
• 期刊: ACS Earth and Space Chemistry
• 影响因子: 3.4
• 作者: Ziying Lei;Nicole E. Olson;Yue Zhang;Yuzhi Chen;A. Lambe;Jing Zhang;Natalie J. White;J. Atkin;M. M. Banaszak Holl-M.;Zhenfa Zhang;A. Gold;J. Surratt;A. Ault

Kinetics and Products of Heterogeneous Hydroxyl Radical Oxidation of Isoprene Epoxydiol-Derived Secondary Organic Aerosol

• DOI: 10.1021/acsearthspacechem.3c00073
• 发表时间: 2023-09
• 期刊: ACS Earth and Space Chemistry
• 影响因子: 3.4
• 作者: Jin Yan;Yue Zhang;Yuzhi Chen;N. C. Armstrong;Nicolas A. Buchenau;Ziying Lei;Yao Xiao;Zhenfa Zhang;A. Lambe;M. N. Chan;Barbara J. Turpin;A. Gold;A. Ault;J. Surratt