Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements

Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) to the observed particulate matter levels have been difficult to quantify. In this study the three-dimensional chemical transport model PMCAMx-...

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Main Authors: Tsimpidi, A. P., Karydis, V. A., Bei, Naifang, Pandis, S. N., Lei, Wenfang, Molina, Luisa Tan, Zavala-Perez, Miguel Angel
Other Authors: Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences
Format: Article
Language:en_US
Published: European Geosciences Union 2011
Online Access:http://hdl.handle.net/1721.1/66520
https://orcid.org/0000-0002-3596-5334
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author Tsimpidi, A. P.
Karydis, V. A.
Bei, Naifang
Pandis, S. N.
Lei, Wenfang
Molina, Luisa Tan
Zavala-Perez, Miguel Angel
author2 Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences
author_facet Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences
Tsimpidi, A. P.
Karydis, V. A.
Bei, Naifang
Pandis, S. N.
Lei, Wenfang
Molina, Luisa Tan
Zavala-Perez, Miguel Angel
author_sort Tsimpidi, A. P.
collection MIT
description Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) to the observed particulate matter levels have been difficult to quantify. In this study the three-dimensional chemical transport model PMCAMx-2008 is used to investigate the temporal and geographic variability of organic aerosol in the Mexico City Metropolitan Area (MCMA) during the MILAGRO campaign that took place in the spring of 2006. The organic module of PMCAMx-2008 includes the recently developed volatility basis-set framework in which both primary and secondary organic components are assumed to be semi-volatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The MCMA emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments. The model predictions are compared with observations from four different types of sites, an urban (T0), a suburban (T1), a rural (T2), and an elevated site in Pico de Tres Padres (PTP). The performance of the model in reproducing organic mass concentrations in these sites is encouraging. The average predicted PM[subscript 1] organic aerosol (OA) concentration in T0, T1, and T2 is 18 μg m[superscript −3], 11.7 μg m[superscript −3], and 10.5 μg m[superscript −3] respectively, while the corresponding measured values are 17.2 μg m[superscript −3], 11 μg m[superscript −3], and 9 μg m[superscript −3]. The average predicted locally-emitted primary OA concentrations, 4.4 μg m[superscript −3] at T0, 1.2 μg m[superscript −3] at T1 and 1.7 μg m[superscript −3] at PTP, are in reasonably good agreement with the corresponding PMF analysis estimates based on the Aerosol Mass Spectrometer (AMS) observations of 4.5, 1.3, and 2.9 μg m[superscript −3] respectively. The model reproduces reasonably well the average oxygenated OA (OOA) levels in T0 (7.5 μg m[superscript −3] predicted versus 7.5 μg m[superscript −3] measured), in T1 (6.3 μg m[superscript −3] predicted versus 4.6 μg m[superscript −3] measured) and in PTP (6.6 μg m[superscript −3] predicted versus 5.9 μg m[superscript −3] measured). The rest of the OA mass (6.1 μg m[superscript −3] and 4.2 μg m[superscript −3] in T0 and T1 respectively) is assumed to originate from biomass burning activities and is introduced to the model as part of the boundary conditions. Inside Mexico City (at T0), the locally-produced OA is predicted to be on average 60 % locally-emitted primary (POA), 6 % semi-volatile (S-SOA) and intermediate volatile (I-SOA) organic aerosol, and 34 % traditional SOA from the oxidation of VOCs (V-SOA). The average contributions of the OA components to the locally-produced OA for the entire modelling domain are predicted to be 32 % POA, 10 % S-SOA and I-SOA, and 58 % V-SOA. The long range transport from biomass burning activities and other sources in Mexico is predicted to contribute on average almost as much as the local sources during the MILAGRO period.
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spelling mit-1721.1/665202024-05-15T03:22:37Z Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements Tsimpidi, A. P. Karydis, V. A. Bei, Naifang Pandis, S. N. Lei, Wenfang Molina, Luisa Tan Zavala-Perez, Miguel Angel Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences Molina, Luisa Tan Zavala, M. Lei, Wenfang Molina, Luisa Tan Bei, Naifang Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) to the observed particulate matter levels have been difficult to quantify. In this study the three-dimensional chemical transport model PMCAMx-2008 is used to investigate the temporal and geographic variability of organic aerosol in the Mexico City Metropolitan Area (MCMA) during the MILAGRO campaign that took place in the spring of 2006. The organic module of PMCAMx-2008 includes the recently developed volatility basis-set framework in which both primary and secondary organic components are assumed to be semi-volatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The MCMA emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments. The model predictions are compared with observations from four different types of sites, an urban (T0), a suburban (T1), a rural (T2), and an elevated site in Pico de Tres Padres (PTP). The performance of the model in reproducing organic mass concentrations in these sites is encouraging. The average predicted PM[subscript 1] organic aerosol (OA) concentration in T0, T1, and T2 is 18 μg m[superscript −3], 11.7 μg m[superscript −3], and 10.5 μg m[superscript −3] respectively, while the corresponding measured values are 17.2 μg m[superscript −3], 11 μg m[superscript −3], and 9 μg m[superscript −3]. The average predicted locally-emitted primary OA concentrations, 4.4 μg m[superscript −3] at T0, 1.2 μg m[superscript −3] at T1 and 1.7 μg m[superscript −3] at PTP, are in reasonably good agreement with the corresponding PMF analysis estimates based on the Aerosol Mass Spectrometer (AMS) observations of 4.5, 1.3, and 2.9 μg m[superscript −3] respectively. The model reproduces reasonably well the average oxygenated OA (OOA) levels in T0 (7.5 μg m[superscript −3] predicted versus 7.5 μg m[superscript −3] measured), in T1 (6.3 μg m[superscript −3] predicted versus 4.6 μg m[superscript −3] measured) and in PTP (6.6 μg m[superscript −3] predicted versus 5.9 μg m[superscript −3] measured). The rest of the OA mass (6.1 μg m[superscript −3] and 4.2 μg m[superscript −3] in T0 and T1 respectively) is assumed to originate from biomass burning activities and is introduced to the model as part of the boundary conditions. Inside Mexico City (at T0), the locally-produced OA is predicted to be on average 60 % locally-emitted primary (POA), 6 % semi-volatile (S-SOA) and intermediate volatile (I-SOA) organic aerosol, and 34 % traditional SOA from the oxidation of VOCs (V-SOA). The average contributions of the OA components to the locally-produced OA for the entire modelling domain are predicted to be 32 % POA, 10 % S-SOA and I-SOA, and 58 % V-SOA. The long range transport from biomass burning activities and other sources in Mexico is predicted to contribute on average almost as much as the local sources during the MILAGRO period. European Union Seventh Framework Programme (European Commission) (Grant agreement no.: 212520) National Science Foundation (U.S.) (ATM 0732598) Molina Center for Energy and the Environment National Science Foundation (U.S.) (ATM 0528227) National Science Foundation (U.S.) (ATM 0810931) 2011-10-20T16:17:20Z 2011-10-20T16:17:20Z 2011-06 2011-05 Article http://purl.org/eprint/type/JournalArticle 1680-7324 1680-7316 http://hdl.handle.net/1721.1/66520 Tsimpidi, A. P. et al. “Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements during MILAGRO.” Atmospheric Chemistry and Physics 11 (2011): 5153-5168. Web. 20 Oct. 2011. https://orcid.org/0000-0002-3596-5334 en_US http://dx.doi.org/10.5194/acp-11-5153-2011 Atmospheric Chemistry and Physics Creative Commons Attribution 3.0 http://creativecommons.org/licenses/by/3.0/ application/pdf European Geosciences Union Copernicus
spellingShingle Tsimpidi, A. P.
Karydis, V. A.
Bei, Naifang
Pandis, S. N.
Lei, Wenfang
Molina, Luisa Tan
Zavala-Perez, Miguel Angel
Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements
title Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements
title_full Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements
title_fullStr Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements
title_full_unstemmed Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements
title_short Sources and production of organic aerosol in Mexico City: insights from the combination of a chemical transport model (PMCAMx-2008) and measurements
title_sort sources and production of organic aerosol in mexico city insights from the combination of a chemical transport model pmcamx 2008 and measurements
url http://hdl.handle.net/1721.1/66520
https://orcid.org/0000-0002-3596-5334
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