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Molecular Corridors and Kinetic Regimes in the Multiphase Chemical Evolution of Secondary Organic Aerosol : Volume 14, Issue 16 (20/08/2014)

By Shiraiwa, M.

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Book Id: WPLBN0003994071
Format Type: PDF Article :
File Size: Pages 19
Reproduction Date: 2015

Title: Molecular Corridors and Kinetic Regimes in the Multiphase Chemical Evolution of Secondary Organic Aerosol : Volume 14, Issue 16 (20/08/2014)  
Author: Shiraiwa, M.
Volume: Vol. 14, Issue 16
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection (Contemporary), Copernicus GmbH
Historic
Publication Date:
2014
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: Copernicus Publications

Citation

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Schilling-Fahnestock, K. A., Seinfeld, J. H., Berkemeier, T., Shiraiwa, M., & Pöschl, U. (2014). Molecular Corridors and Kinetic Regimes in the Multiphase Chemical Evolution of Secondary Organic Aerosol : Volume 14, Issue 16 (20/08/2014). Retrieved from http://www.ebooklibrary.org/


Description
Description: Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany. 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.

Summary
Molecular corridors and kinetic regimes in the multiphase chemical evolution of secondary organic aerosol

Excerpt
Schilling-Fahnestock, K. A., Yee, L. D., Loza, C. L., Coggon, M. M., Schwantes, R., Zhang, X., Dalleska, N. F., and Seinfeld, J. H.: Secondary Organic Aerosol Composition from C12 Alkanes, J. Phys. Chem. A, <a href=http://dx.doi.org/10.1021/jp501779w>doi:10.1021/jp501779w, 2014.; Schobesberger, S., Junninen, H., Bianchi, F., Lonn, G., Ehn, M., Lehtipalo, K., Dommen, J., Ehrhart, S., Ortega, I. K., Franchin, A., Nieminen, T., Riccobono, F., Hutterli, M., Duplissy, J., Almeida, J., Amorim, A., Breitenlechner, M., Downard, A. J., Dunne, E. M., Flagan, R. C., Kajos, M., Keskinen, H., Kirkby, J., Kupc, A., Kuerten, A., Kurten, T., Laaksonen, A., Mathot, S., Onnela, A., Praplan, A. P., Rondo, L., Santos, F. D., Schallhart, S., Schnitzhofer, R., Sipila, M., Tome, A., Tsagkogeorgas, G., Vehkamaki, H., Wimmer, D., Baltensperger, U., Carslaw, K. S., Curtius, J., Hansel, A., Petaja, T., Kulmala, M., Donahue, N. M., and Worsnop, D. R.: Molecular understanding of atmospheric particle formation from sulfuric acid and large oxidized organic molecules, P. Natl. Acad. Sci. USA, 110, 17223–17228, 2013.; Shiraiwa, M., Ammann, M., Koop, T., and Pöschl, U.: Gas uptake and chemical aging of semisolid organic aerosol particles, P. Natl. Acad. Sci. USA, 108, 11003–11008, 2011.; Shiraiwa, M., Pfrang, C., Koop, T., and Pöschl, U.: Kinetic multi-layer model of gas-particle interactions in aerosols and clouds (KM-GAP): linking condensation, evaporation and chemical reactions of organics, oxidants and water, Atmos. Chem. Phys., 12, 2777–2794, <a href=http://dx.doi.org/10.5194/acp-12-2777-2012>doi:10.5194/acp-12-2777-2012, 2012.; Shiraiwa, M. and Seinfeld, J. H.: Equilibration timescale of atmospheric secondary organic aerosol partitioning, Geophys. Res. Lett., 39, L24801, <a href=http://dx.doi.org/10.1029/2012GL054008>doi:10.1029/2012GL054008, 2012.; Shiraiwa, M., Yee, L. D., Schilling, K. A., Loza, C. L., Craven, J. S., Zuend, A., Ziemann, P. J., and Seinfeld, J. H.: Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation, P. Natl. Acad. Sci. USA, 110, 11746–11750, 2013a.; Shiraiwa, M., Zuend, A., Bertram, A. K., and Seinfeld, J. H.: Gas-particle partitioning of atmospheric aerosols: interplay of physical state, non-ideal mixing and morphology, Phys. Chem. Chem. Phys., 15, 11441–11453, 2013b.; Zhang, X., Pandis, S. N., and Seinfeld, J. H.: Diffusion-limited versus quasi-equilibrium aerosol growth, Aerosol Sci. Technol., 46, 874–885, 2012.; Surratt, J. D., Murphy, S. M., Kroll, J. H., Ng, N. L., Hildebrandt, L., Sorooshian, A., Szmigielski, R., Vermeylen, R., Maenhaut, W., Claeys, M., Flagan, R. C., and Seinfeld, J. H.: Chemical composition of secondary organic aerosol formed from the photooxidation of isoprene, J. Phys. Chem. A, 110, 9665–9690, 2006.; Surratt, J. D., Gomez-Gonzalez, Y., Chan, A. W. H., Vermeylen, R., Shahgholi, M., Kleindienst, T. E., Edney, E. O., Offenberg, J. H., Lewandowski, M., Jaoui, M., Maenhaut, W., Claeys, M., Flagan, R. C., and Seinfeld, J. H.: Organosulfate formation in biogenic secondary organic aerosol, J. Phys. Chem. A, 112, 8345–8378, 2008.; Surratt, J. D., Chan, A. W. H., Eddingsaas, N. C., Chan, M. N., Loza, C. L., Kwan, A. J., Hersey, S. P., Flagan, R. C., Wennberg, P. O., and Seinfeld, J. H.: Reactive intermediates revealed in secondary organic aerosol formation from isoprene, P. Natl. Acad. Sci. USA, 107, 6640–6645, 2010.; Trump, E. R. and Donahue, N. M.: Oligomer formation within secondary organic aerosols: equilibrium and dynamic considerations, Atmos. Chem. Phys., 14, 3691–3701, <a href=http://dx.doi.org/10.5194/acp-14-3691-2014>doi:10.5194/acp-14-3691-2014, 2014.; Vaden, T. D., Imre, D., Beranek, J., Shrivastava, M., and Zelenyuk, A.: Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol, P. Natl. Acad. Sci. USA, 108, 2190–2195, 2011.; Virtanen, A.


 

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