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Title: Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California

Abstract

The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 µg m–3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol weremore » identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O/C = 0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O/C = 0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O/C = 0.33; BBOA2: 20 % of total OA, O/C = 0.60) most likely associated with residential space heating from wood combustion, and semivolatile oxygenated OA (SV-OOA; 16 % of total OA, O/C = 0.63) and low-volatility oxygenated OA (LV-OOA; 24 % of total OA, O/C = 0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a previous campaign in winter 2010, most notably that PM1 concentrations were nearly 3 times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 and 12:00 PST. This is an indication that nighttime chemical reactions may have played a more important role in 2013. As solar radiation was stronger in 2013 the higher nitrate and OOA concentrations in 2013 could also be partly due to greater photochemical production of secondary aerosol species. Furthermore, the greater solar radiation and larger range in temperature in 2013 also likely led to both SV-OOA and LV-OOA being observed in 2013 whereas only a single OOA factor was identified in 2010.« less

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ; ; ORCiD logo; ORCiD logo; ; ORCiD logo
Publication Date:
Research Org.:
Univ. of California, Davis, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); National Aeronautics and Space Administration (NASA); California Agricultural Experiment Station; California Air Resources Board; National Science Foundation (NSF) Graduate Research Fellowship; Fundacion Ramon Areces
OSTI Identifier:
1250381
Alternate Identifier(s):
OSTI ID: 1268106
Grant/Contract Number:  
FG02-11ER65293, DE-SC0007178; FG02-11ER65293; SC0007178; 14-307
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 16 Journal Issue: 8; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; san-joaquin valley; secondary organic aerosol; polycyclic aromatic-hydrocarbons; positive matrix factorization; mass-spectrometer data; biomass-burning smoke; new-york-city; high-resolution; particulate matter; air-quality

Citation Formats

Young, Dominique E., Kim, Hwajin, Parworth, Caroline, Zhou, Shan, Zhang, Xiaolu, Cappa, Christopher D., Seco, Roger, Kim, Saewung, and Zhang, Qi. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California. Germany: N. p., 2016. Web. doi:10.5194/acp-16-5427-2016.
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Young, Dominique E., Kim, Hwajin, Parworth, Caroline, Zhou, Shan, Zhang, Xiaolu, Cappa, Christopher D., Seco, Roger, Kim, Saewung, & Zhang, Qi. Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California. Germany. https://doi.org/10.5194/acp-16-5427-2016
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Young, Dominique E., Kim, Hwajin, Parworth, Caroline, Zhou, Shan, Zhang, Xiaolu, Cappa, Christopher D., Seco, Roger, Kim, Saewung, and Zhang, Qi. Mon . "Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California". Germany. https://doi.org/10.5194/acp-16-5427-2016.
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@article{osti_1250381,
title = {Influences of emission sources and meteorology on aerosol chemistry in a polluted urban environment: results from DISCOVER-AQ California},
author = {Young, Dominique E. and Kim, Hwajin and Parworth, Caroline and Zhou, Shan and Zhang, Xiaolu and Cappa, Christopher D. and Seco, Roger and Kim, Saewung and Zhang, Qi},
abstractNote = {The San Joaquin Valley (SJV) in California experiences persistent air-quality problems associated with elevated particulate matter (PM) concentrations due to anthropogenic emissions, topography, and meteorological conditions. Thus it is important to unravel the various sources and processes that affect the physicochemical properties of PM in order to better inform pollution abatement strategies and improve parameterizations in air-quality models. During January and February 2013, a ground supersite was installed at the Fresno–Garland California Air Resources Board (CARB) monitoring station, where comprehensive, real-time measurements of PM and trace gases were performed using instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and an Ionicon proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS) as part of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign. The average submicron aerosol (PM1) concentration was 31.0 µg m–3 and the total mass was dominated by organic aerosols (OA, 55 %), followed by ammonium nitrate (35 %). High PM pollution events were commonly associated with elevated OA concentrations, mostly from primary sources. Organic aerosols had average atomic oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of 0.42, 1.70, and 0.017, respectively. Six distinct sources of organic aerosol were identified from positive matrix factorization (PMF) analysis of the AMS data: hydrocarbon-like OA (HOA; 9 % of total OA, O/C = 0.09) associated with local traffic, cooking OA (COA; 18 % of total OA, O/C = 0.19) associated with food cooking activities, two biomass burning OA (BBOA1: 13 % of total OA, O/C = 0.33; BBOA2: 20 % of total OA, O/C = 0.60) most likely associated with residential space heating from wood combustion, and semivolatile oxygenated OA (SV-OOA; 16 % of total OA, O/C = 0.63) and low-volatility oxygenated OA (LV-OOA; 24 % of total OA, O/C = 0.90) formed via chemical reactions in the atmosphere. Large differences in aerosol chemistry at Fresno were observed between the current campaign (winter 2013) and a previous campaign in winter 2010, most notably that PM1 concentrations were nearly 3 times higher in 2013 than in 2010. These variations were attributed to differences in the meteorological conditions, which influenced primary emissions and secondary aerosol formation. In particular, COA and BBOA concentrations were greater in 2013 than 2010, where colder temperatures in 2013 likely resulted in increased biomass burning activities. The influence from a nighttime formed residual layer that mixed down in the morning was found to be much more intense in 2013 than 2010, leading to sharp increases in ground-level concentrations of secondary aerosol species including nitrate, sulfate, and OOA, in the morning between 08:00 and 12:00 PST. This is an indication that nighttime chemical reactions may have played a more important role in 2013. As solar radiation was stronger in 2013 the higher nitrate and OOA concentrations in 2013 could also be partly due to greater photochemical production of secondary aerosol species. Furthermore, the greater solar radiation and larger range in temperature in 2013 also likely led to both SV-OOA and LV-OOA being observed in 2013 whereas only a single OOA factor was identified in 2010.},
doi = {10.5194/acp-16-5427-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 8,
volume = 16,
place = {Germany},
year = {Mon May 02 00:00:00 EDT 2016},
month = {Mon May 02 00:00:00 EDT 2016}
}
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High resolution PTR-TOF: Quantification and formula confirmation of VOC in real time
journal, June 2010

  • Graus, Martin; Müller, Markus; Hansel, Armin
  • Journal of the American Society for Mass Spectrometry, Vol. 21, Issue 6
  • DOI: 10.1016/j.jasms.2010.02.006

Primary and secondary organic aerosols in Fresno, California during wintertime: Results from high resolution aerosol mass spectrometry: POA AND SOA IN FRESNO IN WINTER
journal, October 2012

  • Ge, Xinlei; Setyan, Ari; Sun, Yele
  • Journal of Geophysical Research: Atmospheres, Vol. 117, Issue D19
  • DOI: 10.1029/2012JD018026

Effect of aqueous-phase processing on aerosol chemistry and size distributions in Fresno, California, during wintertime
journal, January 2012

  • Ge, Xinlei; Zhang, Qi; Sun, Yele
  • Environmental Chemistry, Vol. 9, Issue 3
  • DOI: 10.1071/EN11168
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