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DOI | 10.5194/acp-14-8323-2014 |
Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol | |
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl | |
2014-08-20 | |
发表期刊 | Atmospheric Chemistry and Physics |
出版年 | 2014 |
英文摘要 | The dominant component of atmospheric, organic aerosol is that derived from the oxidation of volatile organic compounds (VOCs), so-called secondary organic aerosol (SOA). SOA consists of a multitude of organic compounds, only a small fraction of which has historically been identified. Formation and evolution of SOA is a complex process involving coupled chemical reaction and mass transport in the gas and particle phases. Current SOA models do not embody the full spectrum of reaction and transport processes, nor do they identify the dominant rate-limiting steps in SOA formation. Based on molecular identification of SOA oxidation products, we show here that the chemical evolution of SOA from a variety of VOC precursors adheres to characteristic "molecular corridors" with a tight inverse correlation between volatility and molar mass. The slope of these corridors corresponds to the increase in molar mass required to decrease volatility by one order of magnitude (-dM / dlogC0). It varies in the range of 10–30 g mol−1, depending on the molecular size of the SOA precursor and the O : C ratio of the reaction products. Sequential and parallel reaction pathways of oxidation and dimerization or oligomerization progressing along these corridors pass through characteristic regimes of reaction-, diffusion-, or accommodation-limited multiphase chemical kinetics that can be classified according to reaction location, degree of saturation, and extent of heterogeneity of gas and particle phases. The molecular corridors and kinetic regimes help to constrain and describe the properties of the products, pathways, and rates of SOA evolution, thereby facilitating the further development of aerosol models for air quality and climate. |
领域 | 地球科学 |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/287993 |
专题 | 地球科学 |
推荐引用方式 GB/T 7714 | M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl. Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol[J]. Atmospheric Chemistry and Physics,2014. |
APA | M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl.(2014).Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol.Atmospheric Chemistry and Physics. |
MLA | M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl."Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol".Atmospheric Chemistry and Physics (2014). |
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