人类活动产生的极低挥发性有机物(ELVOC)控制着大平原南部春季分子集群的增长

IF 3.8 2区 地球科学 Q2 METEOROLOGY & ATMOSPHERIC SCIENCES Journal of Geophysical Research: Atmospheres Pub Date : 2024-10-29 DOI:10.1029/2024JD041212
Manish Shrivastava, Jie Zhang, Rahul A. Zaveri, Bin Zhao, Jeffrey R. Pierce, Samuel E. O’Donnell, Jerome D. Fast, Brian Gaudet, John E. Shilling, Alla Zelenyuk, Benjamin N. Murphy, Havala O. T. Pye, Qi Zhang, Justin Trousdell, Renyi Zhang, Yixin Li, Qi Chen
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引用次数: 0

摘要

新粒子的形成(NPF)通常会推动云凝结核的浓度,而分子团簇的成核过程在不同地区有很大差异。这些直径从 2 纳米到 10 纳米的团聚体的增长通常是由极低挥发性有机蒸汽(ELVOC)的可用性驱动的。虽然人们对生物萜烯氧化形成 ELVOC 的途径了解较多,但对人为有机物氧化形成 ELVOC 的机理途径了解较少。我们整合了测量结果和详细的区域模型模拟,以了解俄克拉荷马州南部大平原观测站的 NPF 和二次有机气溶胶形成过程,并将其与美国东南部阿拉巴马州班克黑德国家森林(BNF)内的一个观测点进行比较。在我们模拟的两个 NPF 事件日期间,预测 SGP 的成核率至少比 BNF 高一个数量级,这主要是由于 BNF 的硫酸 (H2SO4) 浓度较低。在 WRF-Chem 的不同成核机制中,我们发现二甲胺 (DMA) + H2SO4 成核机制在 SGP 占主导地位。我们发现,人为的 ELVOC 对解释在 SGP 观测到的颗粒物生长至关重要。将有机颗粒视为半固体,有机蒸汽在颗粒相中的吸收有很强的扩散限制,这使得模型预测与观测结果更加一致。我们还模拟了在 SGP 站点观测到的两个非 NPF 事件日,结果表明低空云层降低了光化学活动,H2SO4 和人为 ELVOC 浓度也相应降低,从而解释了为什么没有出现 NPF。
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Anthropogenic Extremely Low Volatility Organics (ELVOCs) Govern the Growth of Molecular Clusters Over the Southern Great Plains During the Springtime

New particle formation (NPF) often drives cloud condensation nuclei concentrations and the processes governing nucleation of molecular clusters vary substantially in different regions. The growth of these clusters from ∼2 to >10 nm diameters is often driven by the availability of extremely low volatility organic vapors (ELVOCs). Although the pathways to ELVOC formation from the oxidation of biogenic terpenes are better understood, the mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are less well understood. We integrate measurements and detailed regional model simulations to understand the processes governing NPF and secondary organic aerosol formation at the Southern Great Plain (SGP) observatory in Oklahoma and compare these with a site within the Bankhead National Forest (BNF) in Alabama, southeast USA. During our two simulated NPF event days, nucleation rates are predicted to be at least an order of magnitude higher at SGP compared to BNF largely due to lower sulfuric acid (H2SO4) concentrations at BNF. Among the different nucleation mechanisms in WRF-Chem, we find that the dimethylamine (DMA) + H2SO4 nucleation mechanism dominates at SGP. We find that anthropogenic ELVOCs are critical for explaining the growth of particles observed at SGP. Treating organic particles as semisolid, with strong diffusion limitations for organic vapor uptake in the particle phase, brings model predictions into closer agreement with observations. We also simulate two non-NPF event days observed at the SGP site and show that low-level clouds reduce photochemical activity with corresponding reductions in H2SO4 and anthropogenic ELVOC concentrations, thereby explaining the lack of NPF.

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来源期刊
Journal of Geophysical Research: Atmospheres
Journal of Geophysical Research: Atmospheres Earth and Planetary Sciences-Geophysics
CiteScore
7.30
自引率
11.40%
发文量
684
期刊介绍: JGR: Atmospheres publishes articles that advance and improve understanding of atmospheric properties and processes, including the interaction of the atmosphere with other components of the Earth system.
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