Formation and Evolution of Atmospheric Brown Carbon from Nitrate Radical Initiated Oxidation of Heterocyclic Volatile Organic Compounds

杂环挥发性有机化合物硝酸根引发氧化导致大气棕碳的形成与演化

• 批准号: 1953905
• 负责人: Ying-Hsuan Lin
• 金额: $ 69.93万
• 依托单位: University of California-Riverside
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-07-01 至 2024-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1953905&HistoricalAwards=false
• 关键词: Formation; Evolution; Atmospheric; Brown; Carbon

Brown carbon (BrC) particles in biomass burning plumes affect climate through their interaction with radiation and Earth’s energy budget, yet, little is known about their formation and radiative characteristics. In this multi-PI project, atmospheric formation and transformation processes of BrC particles are studied in systematic laboratory experiments using sophisticated analytical tools. Resulting new mechanistic information will aid in the interpretation of field observations and inform predictive climate models. The project aims at increasing understanding of mechanisms of atmospheric oxidation of heterocyclic volatile organic carbons (VOCs) as sources of brown carbon (BrC) secondary organic aerosols (SOA). Systematic laboratory chamber and flow reactor experiments will be carried out that mimic nighttime conditions in which relevant VOCs are oxidized initially with nitrate radical (NO3) and subsequently aged diurnally with NO3 and hydroxyl (OH) radicals. A suite of on- and off-line state-of-the-art instruments will be employed to characterize particles’ physical and chemical properties, including size, optical parameters, molecular composition, and functional groups. In addition, a multiphase kinetic model will be developed with the data obtained from compositional measurements. The outcome of this work will aid in the interpretation of observations made in complex real biomass burning systems and provide fundamental mechanistic information that can be incorporated into larger scale climate models. Three graduate students will carry out the bulk of the laboratory work, and a number of undergraduate students from underrepresented populations will be recruited from existing programs on the PIs campus. Outreach activities include engagement with local high schools.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.

生物质燃烧羽流中的棕碳（BrC）颗粒通过与辐射和地球能量收支的相互作用影响气候，但人们对它们的形成和辐射特性知之甚少。在这个多PI项目中，使用先进的分析工具在系统的实验室实验中研究了大气中BrC颗粒的形成和转化过程。由此产生的新的机械信息将有助于解释现场观测和通知预测气候模型。该项目旨在加深对杂环挥发性有机碳（VOCs）作为棕色碳（BrC）次级有机气溶胶（SOA）来源的大气氧化机制的理解。将进行系统的实验室和流动反应器实验，模拟夜间条件，其中相关的挥发性有机化合物最初与硝酸根（NO3）氧化，随后与NO3和羟基（OH）自由基日龄。将采用一套在线和离线最先进的仪器来表征颗粒的物理和化学性质，包括尺寸、光学参数、分子组成和官能团。此外，多相动力学模型将开发与从成分测量获得的数据。这项工作的成果将有助于解释在复杂的真实的生物质燃烧系统中所作的观测，并提供可纳入更大尺度气候模型的基本机械信息。三名研究生将进行大部分的实验室工作，一些来自代表性不足的人口的本科生将从PI校园的现有项目中招募。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值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

Effects of Nitrate Radical Levels and Pre-Existing Particles on Secondary Brown Carbon Formation from Nighttime Oxidation of Furan

• DOI: 10.1021/acsearthspacechem.2c00244
• 发表时间: 2022-10-18
• 期刊: ACS EARTH AND SPACE CHEMISTRY
• 影响因子: 3.4
• 作者: Chen, Kunpeng;Mayorga, Raphael;Lin, Ying-Hsuan
• 通讯作者: Lin, Ying-Hsuan

Chemical Structure Regulates the Formation of Secondary Organic Aerosol and Brown Carbon in Nitrate Radical Oxidation of Pyrroles and Methylpyrroles

化学结构调节吡咯和甲基吡咯硝酸盐自由基氧化中二次有机气溶胶和棕碳的形成

• DOI: 10.1021/acs.est.2c02345
• 发表时间: 2022
• 期刊: Environmental Science & Technology
• 影响因子: 11.4
• 作者: Mayorga, Raphael;Chen, Kunpeng;Raeofy, Nilofar;Woods, Megan;Lum, Michael;Zhao, Zixu;Zhang, Wen;Bahreini, Roya;Lin, Ying-Hsuan;Zhang, Haofei
• 通讯作者: Zhang, Haofei

Formation of secondary organic aerosol from nitrate radical oxidation of phenolic VOCs: Implications for nitration mechanisms and brown carbon formation

• DOI: 10.1016/j.atmosenv.2020.117910
• 发表时间: 2021-01
• 期刊: Atmospheric Environment
• 影响因子: 5
• 作者: Raphael Mayorga;Zixu Zhao;Haofei Zhang

Solvent effects on chemical composition and optical properties of extracted secondary brown carbon constituents

• DOI: 10.1080/02786826.2022.2100734
• 发表时间: 2022-07-17
• 期刊: AEROSOL SCIENCE AND TECHNOLOGY
• 影响因子: 5.2
• 作者: Chen, Kunpeng;Raeofy, Nilofar;Lin, Ying-Hsuan
• 通讯作者: Lin, Ying-Hsuan