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Explicit Modeling of Organic Chemistry and Secondary Organic Aerosol Partitioning for Mexico City and Its Outflow Plume : Volume 11, Issue 6 (20/06/2011)

By Lee-taylor, J.

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Book Id: WPLBN0003985370
Format Type: PDF Article :
File Size: Pages 58
Reproduction Date: 2015

Title: Explicit Modeling of Organic Chemistry and Secondary Organic Aerosol Partitioning for Mexico City and Its Outflow Plume : Volume 11, Issue 6 (20/06/2011)  
Author: Lee-taylor, J.
Volume: Vol. 11, Issue 6
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection (Contemporary), Copernicus GmbH
Historic
Publication Date:
2011
Publisher: Copernicus Gmbh, Göttingen, Germany

Citation

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Madronich, S., Camredon, M., Aumont, B., Lee-Taylor, J., Apel, E., Hodzic, A.,...Tyndall, G. S. (2011). Explicit Modeling of Organic Chemistry and Secondary Organic Aerosol Partitioning for Mexico City and Its Outflow Plume : Volume 11, Issue 6 (20/06/2011). Retrieved from http://worldlibrary.in/


Description
Description: National Center for Atmospheric Research, Boulder, Colorado, USA. The evolution of organic aerosols (OA) in Mexico City and its outflow is investigated with the nearly explicit gas phase photochemistry model GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere), wherein precursor hydrocarbons are oxidized to numerous intermediate species for which vapor pressures are computed and used to determine gas/particle partitioning in a chemical box model. Precursor emissions included observed C3–10 alkanes, alkenes, and light aromatics, as well as larger n-alkanes (up to C25) not directly observed but estimated by scaling to particulate emissions according to their volatility. Conditions were selected for comparison with observations made in March 2006 (MILAGRO). The model successfully reproduces the magnitude and diurnal shape for both primary (POA) and secondary (SOA) organic aerosols, with POA peaking in the early morning at 15–20 μg m−3, and SOA peaking at 10–15 μg m−3 during mid-day. The majority (≥75 %) of the model SOA stems from the large n-alkanes, with the remainder mostly from the light aromatics. Simulated OA elemental composition reproduces observed H/C and O/C ratios reasonably well, although modeled ratios develop more slowly than observations suggest. SOA chemical composition is initially dominated by δ-hydroxy ketones and nitrates from the large alkanes, with contributions from peroxy acyl nitrates and, at later times when NOx is lower, organic hydroperoxides. The simulated plume-integrated OA mass continues to increase for several days downwind despite dilution-induced particle evaporation, since oxidation chemistry leading to SOA formation remains strong. In this model, the plume SOA burden several days downwind exceeds that leaving the city by a factor of >3. These results suggest significant regional radiative impacts of SOA.

Summary
Explicit modeling of organic chemistry and secondary organic aerosol partitioning for Mexico City and its outflow plume

Excerpt
Aumont, B., Camredon, M., Valorso, R., Lee-Taylor, J., and Madronich, S.: Development of Systematic Reduction Techniques to Describe the SOA/VOC/NOx/O3 System, in: Atmospheric Chemical Mechanisms Conference, Air Quality Research Center, UC Davis, CA, 10–12 December 2008, 2008.; Barley, M. H. and McFiggans, G.: The critical assessment of vapour pressure estimation methods for use in modelling the formation of atmospheric organic aerosol, Atmos. Chem. Phys., 10, 749–767, doi:10.5194/acp-10-749-2010, 2010.; Barsanti, K. C. and Pankow, J. F.: Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions – Part 1: aldehydes and ketones, Atmos. Environ., 38, 4371–4382, doi:10.1016/j.atmosenv.2004.03.035, 2004.; Blake, D. R. and Rowland, F. S.: Urban leakage of liquefied petroleum gas and its impact on Mexico-City air-quality, Science, 269, 953–956, 1995.; Aiken, A. C., Decarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffman, J. A., Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Sun, Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratna, M. R., Onasch, T. B., Alfarra, M. R., Prevot, A. S. H., Dommen, J., Duplissy, J., Metzger, A., Baltensperger, U., and Jimenez, J. L.: O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry, Environ. Sci. Technol., 42, 4478–4485 doi:10.1021/es703009q, 2008.; Aiken, A. C., Salcedo, D., Cubison, M. J., Huffman, J. A., DeCarlo, P. F., Ulbrich, I. M., Docherty, K. S., Sueper, D., Kimmel, J. R., Worsnop, D. R., Trimborn, A., Northway, M., Stone, E. A., Schauer, J. J., Volkamer, R. M., Fortner, E., de Foy, B., Wang, J., Laskin, A., Shutthanandan, V., Zheng, J., Zhang, R., Gaffney, J., Marley, N. A., Paredes-Miranda, G., Arnott, W. P., Molina, L. T., Sosa, G., and Jimenez, J. L.: Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 1: Fine particle composition and organic source apportionment, Atmos. Chem. Phys., 9, 6633–6653, doi:10.5194/acp-9-6633-2009, 2009.; Aumont, B., Madronich, S., Bey, I., and Tyndall, G. S.: Contribution of secondary VOC to the composition of aqueous atmospheric particles: a modeling approach, J. Atmos. Chem., 35, 59–75, 2000.; Aumont, B., Szopa, S., and Madronich, S.: Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach, Atmos. Chem. Phys., 5, 2497–2517, doi:10.5194/acp-5-2497-2005, 2005.; Apel, E.&

 

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