Top-Down Constraints on North American Biogenic Volatile Organic Compounds (VOC) Emissions From Tall Tower Measurements and Lagrangian Particle Dispersion Modeling

高塔测量和拉格朗日粒子分散模型对北美生物挥发性有机化合物 (VOC) 排放的自上而下约束

• 批准号: 0937004
• 负责人: Dylan Millet
• 金额: $ 46.22万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2009
• 资助国家: 美国
• 起止时间: 2009-10-01 至 2013-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0937004&HistoricalAwards=false
• 关键词: Top; Down; Constraints; North; American

Atmospheric volatile organic compounds (VOCs) are precursors of tropospheric ozone, carbon monoxide (CO), formaldehyde, and organic aerosol, and play a central role in hydrogen oxides (HOx) and nitrogen oxides (NOy) cycling. Terrestrial ecosystems are the dominant source of VOCs to the global atmosphere. This research will advance scientific understanding of biogenic VOC (BVOC) emissions and their atmospheric effects by addressing the following core questions: What is the landscape to regional-scale distribution of BVOC fluxes, and how do they respond to environmental forcing and phenology? What is the seasonal impact of BVOCs on CO and other key atmospheric species? What roles do BVOCs play during spring and fall in driving a chemical transition between NOx and VOC-limited regimes for ozone production? The research applies a new measurement-model approach linking tall tower BVOC measurements with Lagrangian and inverse modeling. Work will focus on isoprene, methanol, and acetone - three of the most ubiquitous and important BVOCs. Specific tasks will include: 1) Measure BVOC and CO concentrations at an Ameriflux tall tower (244 m) in the US Midwest. Measurements will span two full annual cycles. 2) Analyze the VOC concentrations and variability in relation to upstream sources, landcover, and season. This unique dataset will yield new insights into the controls on atmospheric VOC abundance and chemical impacts on timescales from minutes to years. 3) Relate the measurements quantitatively to regional sources using the Stochastic Time- Inverted Lagrangian Transport (STILT) model and state-of-science emission inventories. 4) Apply a formal Bayesian inverse analysis to place new constraints on landscape-to-regional scale (~ 100 - 1,000 km) BVOC sources. 5) Explore the seasonal dependence of emissions and the resulting photochemical effects on CO and other key species.Broader impact and outreach components of the work include: 1) Broadening the participation of underrepresented students in Earth Science research through a partnership with the McNair Scholars program; 2) Training graduate students in cutting-edge atmospheric chemistry measurement and modeling tools; 3) Developing a new model-measurement tool that should be broadly useful to the scientific community; 4) Active dissemination of scientific findings through conference presentations and scientific publications. Finalized data will be made public and readily available online.

大气挥发性有机化合物 (VOC) 是对流层臭氧、一氧化碳 (CO)、甲醛和有机气溶胶的前体，在氢氧化物 (HOx) 和氮氧化物 (NOy) 循环中发挥核心作用。 陆地生态系统是全球大气中挥发性有机化合物的主要来源。 这项研究将通过解决以下核心问题，促进对生物 VOC (BVOC) 排放及其大气影响的科学认识：BVOC 通量的区域尺度分布情况如何，以及它们如何响应环境强迫和物候？ BVOC 对 CO 和其他主要大气物种的季节性影响是什么？ BVOC 在春季和秋季在推动臭氧生产的 NOx 和 VOC 限制状态之间的化学转变方面发挥什么作用？ 该研究采用了一种新的测量模型方法，将高塔 BVOC 测量与拉格朗日和反演建模联系起来。 工作重点是异戊二烯、甲醇和丙酮——三种最普遍、最重要的 BVOC。 具体任务包括： 1) 测量美国中西部 Ameriflux 高塔 (244 m) 的 BVOC 和 CO 浓度。 测量将跨越两个完整的年度周期。 2) 分析与上游来源、土地覆盖和季节相关的 VOC 浓度和变化。 这个独特的数据集将为控制大气 VOC 丰度和化学影响（从几分钟到几年的时间尺度）提供新的见解。 3) 使用随机时间反演拉格朗日传输 (STILT) 模型和最新的排放清单将测量结果与区域源定量关联。 4) 应用正式的贝叶斯逆分析对景观到区域尺度（约 100 - 1,000 公里）BVOC 源施加新的约束。 5) 探索排放的季节性依赖性以及由此产生的对二氧化碳和其他关键物种的光化学效应。该工作的更广泛影响和外展部分包括： 1) 通过与麦克奈尔学者计划的合作，扩大代表性不足的学生对地球科学研究的参与; 2）培养研究生使用尖端大气化学测量和建模工具； 3）开发一种对科学界广泛有用的新模型测量工具； 4) 通过会议报告和科学出版物积极传播科学发现。 最终数据将公开并可在线获取。