RAPID: Online Single-particle Measurements of the Chemical Composition, Mixing State, and Ice Nuclei Residues During the FLAME IV Biomass Burning Experiment

RAPID：FLAME IV 生物质燃烧实验期间化学成分、混合状态和冰核残留物的在线单粒子测量

• 批准号: 1256042
• 负责人: Ryan Sullivan
• 金额: $ 2.49万
• 依托单位: Carnegie-Mellon University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-10-01 至 2013-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1256042&HistoricalAwards=false
• 关键词: RAPID; Online; Single; particle; Measurements

This RAPID project involves performing online single-particle mass spectrometry (SP-MS) measurements of the chemical composition and mixing state of biomass particles during the fourth Fire Lab At Missoula Experiment (FLAME IV). FLAME IV affords a unique and important opportunity to better understand the evolution of biomass smoke more completely than is possible in the Carnegie-Mellon University (CMU) laboratory, by taking advantage of the collaborative simultaneous measurements conducted by a wide range of scientists. The SP-MS will determine how the aerosol mixing state evolves as the biomass smoke is photochemically aged in a novel twin environmental chamber system. The chambers will be filled with combustion smoke generated from a variety of globally relevant biomass fuels, and diluted to atmospheric concentrations. Atmospheric photochemistry will be simulated in the chambers for several hours using photo-simulator lights and the optional addition of oxidants such as hydroxyl radical and nitrogen oxides. The twin chamber design will provide an unperturbed control aerosol system to which aerosols in the perturbed chamber can be compared at any time during the multi-hour long experiments. Through tandem experiments with FLAME IV participants from Colorado State University, the SP-MS will also determine the chemical composition of ice nuclei present in fresh and aged biomass burning smoke. A novel suite of gas and aerosol instruments will be used to thoroughly characterize the biomass aerosol prior to, during, and after simulated photochemistry. The instrument package includes a High-Resolution Time-Of-Flight Aerosol Mass Spectrometer, Proton-Transfer-Reaction Mass Spectrometer, and a new single-particle mass spectrometer. This will be the first deployment of this new Laser Ablation Aerosol Particle Time-Of-Flight (LAAP-TOF) mass spectrometer in any collaborative experimental or field campaign. The LAAP-TOF will allow better understanding to be gained of the variations in individual particle composition and mixing state for the different fuels tested, how this mixing state evolves during photo-oxidation, and what role this mixing state might play in the partitioning of organic carbon between the gas and particle phases.The research cuts across multiple disciplines including chemistry, combustion, air quality engineering, atmospheric science, and climate change. Thus, this research will have immediate impacts on a wide range of interdisciplinary fields including forest management, atmospheric chemistry, cloud microphysics, and biogeochemistry. The project will compose a significant portion of at least two graduate student Ph.D. dissertations, and the research of one post-doctoral associate. The collaborative and multi-disciplinary nature of the FLAME IV experiment will provide our participants with the unique opportunity to work alongside a wider range of scientists than otherwise possible during their research at CMU.

该RAPID项目涉及在第四次米苏拉实验（FLAME IV）火灾实验室期间对生物质颗粒的化学组成和混合状态进行在线单颗粒质谱（SP-MS）测量。FLAME IV提供了一个独特而重要的机会，通过利用由广泛的科学家进行的协作同步测量，可以比卡内基-梅隆大学（CMU）实验室更全面地了解生物质烟雾的演变。SP-MS将确定气溶胶混合状态如何演变为生物质烟雾光化学老化在一个新的双环境室系统。燃烧室将充满各种全球相关生物质燃料产生的燃烧烟雾，并稀释至大气浓度。大气光化学将在室内模拟数小时，使用光模拟器灯和可选的氧化剂，如羟基自由基和氮氧化物。双室设计将提供一个不受干扰的控制气溶胶系统，可以在多小时长的实验期间的任何时间比较受干扰室中的气溶胶。通过与来自科罗拉多州立大学的FLAME IV参与者的串联实验，SP-MS还将确定新鲜和老化生物质燃烧烟雾中存在的冰核的化学成分。一套新的气体和气溶胶仪器将被用来彻底表征生物质气溶胶之前，期间和之后模拟光化学。仪器包包括一个高分辨率飞行时间气溶胶质谱仪，质子转移反应质谱仪，和一个新的单粒子质谱仪。这将是这种新型激光烧蚀气溶胶粒子飞行时间（LAAP-TOF）质谱仪在任何合作实验或现场活动中的首次部署。LAAP-TOF将有助于更好地了解所测试的不同燃料的单个颗粒成分和混合状态的变化，这种混合状态在光氧化过程中如何演变，以及这种混合状态在气相和颗粒相之间的有机碳分配中可能发挥什么作用。该研究跨越多个学科，包括化学，燃烧，空气质量工程，大气科学，和气候变化 因此，这项研究将对森林管理、大气化学、云微物理学和地球化学等广泛的跨学科领域产生直接影响。 该项目将构成至少两个研究生博士的重要部分。论文，和一个博士后助理的研究。FLAME IV实验的协作和多学科性质将为我们的参与者提供独特的机会，与CMU研究期间可能的更广泛的科学家一起工作。

项目成果

Production of Secondary Organic Aerosol During Aging of Biomass Burning Smoke From Fresh Fuels and Its Relationship to VOC Precursors

• DOI: 10.1029/2018jd029068
• 发表时间: 2019-03-27
• 期刊: JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
• 影响因子: 4.4
• 作者: Ahern, A. T.;Robinson, E. S.;Donahue, N. M.
• 通讯作者: Donahue, N. M.