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Parameterising Secondary Organic Aerosol from Α-pinene Using a Detailed Oxidation and Aerosol Formation Model : Volume 11, Issue 8 (18/08/2011)

By Ceulemans, K.

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Book Id: WPLBN0003993332
Format Type: PDF Article :
File Size: Pages 48
Reproduction Date: 2015

Title: Parameterising Secondary Organic Aerosol from Α-pinene Using a Detailed Oxidation and Aerosol Formation Model : Volume 11, Issue 8 (18/08/2011)  
Author: Ceulemans, K.
Volume: Vol. 11, Issue 8
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection (Contemporary), Copernicus GmbH
Historic
Publication Date:
2011
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: Copernicus Publications

Citation

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Ceulemans, K., Compernolle, S., & Müller, J. (2011). Parameterising Secondary Organic Aerosol from Α-pinene Using a Detailed Oxidation and Aerosol Formation Model : Volume 11, Issue 8 (18/08/2011). Retrieved from http://worldebooklibrary.com/


Description
Description: Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, Belgium. A new 10-product parameter model for α-pinene secondary organic aerosol (SOA) is presented, based on simulations with the detailed model BOREAM (Biogenic hydrocarbon Oxidation and Related Aerosol formation Model). The parameterisation takes into account the influence of temperature, type of oxidant, NOx-regime, photochemical ageing and water uptake, and is suitable for use in global chemistry transport models. BOREAM is validated against recent photooxidation smog chamber experiments, for which it reproduces SOA yields to within a factor of 2 in most cases. In the simple chemical mechanism of the parameter model, oxidation of α-pinene generates peroxy radicals, which, upon reaction with NO or HO2, yield products corresponding to high or low-NOx conditions, respectively. The model parameters – i.e. the temperature-dependent stoichiometric coefficients and partitioning coefficients of the 10 semi-volatile products – are obtained from simulations with BOREAM, including a prescribed diurnal cycle for the radiation, oxidant and emission levels, as well as a deposition sink for the particulate and gaseous products. The effects of photooxidative ageing are implicitly included in the parameterisation, since it is based on near-equilibrium SOA concentrations, obtained through simulations of a two-week period. Modelled SOA mass yields are about ten times higher in low-NOx than in high-NOx conditions, with yields of about 50 % in the low-NOx OH-initiated oxidation of α-pinene, considerably more than in previous parameterisations based on smog chamber experiments. The parameterisation is only moderately sensitive to the assumed oxidant levels. However, photolysis of species in the particulate phase is found to strongly reduce SOA yields. Water uptake is parameterised using fitted activity coefficients, resulting in a good agreement with the full model.

Summary
Parameterising secondary organic aerosol from Α-pinene using a detailed oxidation and aerosol formation model

Excerpt
Capouet, M. and M{ü}ller, J.-F.: A group contribution method for estimating the vapour pressures of {α}-pinene oxidation products, Atmos. Chem. Phys., 6, 1455–1467, doi:10.5194/acp-6-1455-2006, 2006.; Capouet, M., Peeters, J., Nozière, B., and Müller, J.-F.: {α}-pinene oxidation by {OH}: simulations of laboratory experiments, Atmos. Chem. Phys., 4, 2285–2311, doi:10.5194/acp-4-2285-2004, 2004.; Capouet, M., M{ü}ller, J.-F., Ceulemans, K., Compernolle, S., Vereecken, L., and Peeters, J.: Modeling aerosol formation in {α}-pinene photooxidation experiments, J. Geophys. Res., 113, D02308, doi:10.1029/2007JD008995, 2008.; Carlton, A. G., Bhave, P. V., Napelenok, S. L., Edney, E. O., Sarwar, G., Pinder, R. W., Pouliot, G. A., and Houyoux, M.: Model representation of secondary organic aerosol in CMAQv4.7, Environ. Sci. Technol., 44, 8553–8560, 2010.; Carter, W. P. L.: Documentation of the SAPRC-99 chemical mechanism for VOC reactivity assessment, final report to California Resources Board, contracts 92-329 and 95-308, Tech. rep., Air Pollut. Res. Cent.for Environ. Res. and Technol., Univ. of California, Riverside, California, USA, http://.www.cert.ucr.edu/ carter/reactdat.htm, 2000.; Ceulemans, K., Compernolle, S., Peeters, J., and M{ü}ller, J.-F.: Evaluation of a detailed model of secondary organic aerosol formation from alpha-pinene against dark ozonolysis experiments, Atmos. Environ., 40, 5434–5442, 2010.; Chung, S. H. and Seinfeld, J. H.: Global distribution and climate forcing of carbonaceous aerosols, J. Geophys. Res., 107, 4407, doi:10.1029/2001JD001397, 2002.; Cocker III, D. R., Clegg, S. L., Flagan, R. C., and Seinfeld, J. H.: The effect of water on gas-particle partitioning of secondary organic aerosol. Part {I}: {α}-pinene/ozone system, Atmos. Environ., 35, 6049–6072, 2001.; Compernolle, S., Ceulemans, K., and M{ü}ller, J.-F.: Influence of non-ideality on condensation to aerosol, Atmos. Chem. Phys., 9, 1325–1337, doi:10.5194/acp-9-1325-2009, 2009.; Engelhart, G. J., Hildebrandt, L., Kostenidou, E., Mihalopoulos, N., Donahue, N. M., and Pandis, S. N.: Water content of aged aerosol, Atmos. Chem. Phys., 11, 911–920, doi:10.5194/acp-11-911-2011, 2011.; Farina, S. C., Adams, P. J., and Pandis, S. N.: Modeling global secondary organic aerosol formation and processing with the volatility basis set: Implications for anthropogenic secondary organic aerosol, J. Geophys. Res., 115, D09202, doi:10.1029/2009JD013046, 2010.; Fredenslund, A., Jones, R. L., and Prausnitz, J. M.: Group-contribution estimation of activity-coefficients in nonideal liquid-mixtures, AIChE J., 21, 1086–1099, 1975.; Griffin, R. J., Flagan, R. C., and Seinfeld, J. H.: Organic aerosol formation from the oxidation of biogenic hydrocarbons, J. Geophys. Res., 104, 3555–3567, doi:10.1029/1998JD100049, 1999.; Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, T. F., Monod, A., Pr�v�t, A. S. H., Seinfel

 

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