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Title: 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

Abstract

Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM{sub 2.5} chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assignmore » the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM{sub 2.5} emissions by a factor of {approx}4, and it is {approx}16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is at least an order-of-magnitude larger than in the inventory.« less

Authors:
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Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE SC OFFICE OF SCIENCE (SC)
OSTI Identifier:
1040208
Report Number(s):
BNL-90617-2009-JA
Journal ID: ISSN 1680-7316; R&D Project: 2011-BNL-EE630EECA-Budg; KP1205030; TRN: US201210%%390
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Journal Name:
Atmospheric Chemistry and Physics
Additional Journal Information:
Journal Volume: 9; Journal Issue: 17; Journal ID: ISSN 1680-7316
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; 54 ENVIRONMENTAL SCIENCES; ACETONITRILE; AEROSOLS; AMINES; BIOMASS; FACTORIZATION; FORESTS; MASS BALANCE; MASS SPECTROMETERS; MASS SPECTROSCOPY; MEXICO; NITROGEN; PLUMES; RESOLUTION; SPECTRA

Citation Formats

Aiken, A C, Wang, J, 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, 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. United States: N. p., 2009. Web. doi:10.5194/acp-9-6633-2009.
Aiken, A C, Wang, J, 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, Laskin, A, Shutthanandan, V, Zheng, J, Zhang, R, Gaffney, J, Marley, N A, Paredes-Miranda, G, Arnott, W P, Molina, L T, Sosa, G, & 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. United States. https://doi.org/10.5194/acp-9-6633-2009
Aiken, A C, Wang, J, 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, 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. 2009. "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". United States. https://doi.org/10.5194/acp-9-6633-2009.
@article{osti_1040208,
title = {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},
author = {Aiken, A C and Wang, J and Salcedo, D and Cubison, M J and Huffman, J A and DeCarlo, P F and Ulbrich, I M and Docherty, K S and Sueper, D and Kimmel, J R and Worsnop, D R and Trimborn, A and Northway, M and Stone, E A and Schauer, J J and Volkamer, R M and Fortner, E and de Foy, B and Laskin, A and Shutthanandan, V and Zheng, J and Zhang, R and Gaffney, J and Marley, N A and Paredes-Miranda, G and Arnott, W P and Molina, L T and Sosa, G and Jimenez, J L},
abstractNote = {Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM{sub 2.5} chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assign the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM{sub 2.5} emissions by a factor of {approx}4, and it is {approx}16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is at least an order-of-magnitude larger than in the inventory.},
doi = {10.5194/acp-9-6633-2009},
url = {https://www.osti.gov/biblio/1040208}, journal = {Atmospheric Chemistry and Physics},
issn = {1680-7316},
number = 17,
volume = 9,
place = {United States},
year = {2009},
month = {9}
}