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Title: On the contribution of nocturnal heterogeneous reactive nitrogen chemistry to particulate matter formation during wintertime pollution events in Northern Utah

Abstract

Mountain basins in Northern Utah, including the Salt Lake Valley (SLV), suffer from wintertime air pollution events associated with stagnant atmospheric conditions. During these events, fine particulate matter concentrations (PM 2.5) can exceed national ambient air quality standards. Previous studies in the SLV have found that PM 2.5 is primarily composed of ammonium nitrate (NH 4NO 3), formed from the condensation of gas-phase ammonia (NH 3) and nitric acid (HNO 3).Additional studies in several western basins, including the SLV, have suggested that production of HNO 3 from nocturnal heterogeneous N 2O 5 uptake is the dominant source of NH 4NO 3 during winter. The rate of this process, however, remains poorly quantified, in part due to limited vertical measurements above the surface, where this chemistry is most active. The 2017 Utah Winter Fine Particulate Study(UWFPS) provided the first aircraft measurements of detailed chemical composition during wintertime pollution events in the SLV. Coupled with ground-based observations, analyses of day- and nighttime research flights confirm that PM 2.5 during wintertime pollution events is principally composed of NH 4NO 3, limited by HNO 3. Here, observations and box model analyses assess the contribution of N 2O 5 uptake to nitrate aerosol during pollution events using the $$\mathrm{NO^{-}_{3}}$$ production rate, N 2O 5 heterogeneous uptake coefficient ( γ(N 2O 5)), and production yield of ClNO 2 ( φ(ClNO 2)), which had medians of 1.6 µg m -3 h -1, 0.076,and 0.220, respectively. While fit values of γ(N 2O 5) maybe biased high by a potential under-measurement in aerosol surface area,other fit quantities are unaffected. Lastly, additional model simulations suggest nocturnal N 2O 5 uptake produces between 2.4 and 3.9 µg m -3 of nitrate per day when considering the possible effects of dilution. This nocturnal production is sufficient to account for 52 %–85 %of the daily observed surface-level buildup of aerosol nitrate, though accurate quantification is dependent on modeled dilution, mixing processes,and photochemistry.

Authors:
 [1];  [2];  [3];  [2];  [2]; ORCiD logo [4];  [5];  [6];  [6]; ORCiD logo [7];  [8];  [9];  [10]
  1. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Chemical Sciences Division; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences and Dept. of Chemistry; Dalhousie Univ., Halifax, NS (Canada). Dept. of Physics and Atmospheric Science
  2. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Chemical Sciences Division; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences
  3. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Chemical Sciences Division; Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences; California Air Resources Board, Sacramento, CA (United States)
  4. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Chemical Sciences Division
  5. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Science; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). ARM Aerial Facility
  6. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Science
  7. Univ. of Toronto, Toronto, ON (Canada). Dept. of Chemistry; York Univ., Toronto, ON (Canada). Dept. of Chemistry
  8. Univ. of Toronto, Toronto, ON (Canada). Dept. of Chemistry
  9. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Atmospheric Sciences; Chevron Corporation, Houston, TX (United States)
  10. National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Chemical Sciences Division; Univ. of Colorado, Boulder, CO (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1571482
Report Number(s):
PNNL-SA-147344
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 19; Journal Issue: 14; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

McDuffie, Erin E., Womack, Caroline C., Fibiger, Dorothy L., Dube, William P., Franchin, Alessandro, Middlebrook, Ann M., Goldberger, Lexie, Lee, Ben H., Thornton, Joel A., Moravek, Alexander, Murphy, Jennifer G., Baasandorj, Munkhbayar, and Brown, Steven S. On the contribution of nocturnal heterogeneous reactive nitrogen chemistry to particulate matter formation during wintertime pollution events in Northern Utah. United States: N. p., 2019. Web. doi:10.5194/acp-19-9287-2019.
McDuffie, Erin E., Womack, Caroline C., Fibiger, Dorothy L., Dube, William P., Franchin, Alessandro, Middlebrook, Ann M., Goldberger, Lexie, Lee, Ben H., Thornton, Joel A., Moravek, Alexander, Murphy, Jennifer G., Baasandorj, Munkhbayar, & Brown, Steven S. On the contribution of nocturnal heterogeneous reactive nitrogen chemistry to particulate matter formation during wintertime pollution events in Northern Utah. United States. doi:10.5194/acp-19-9287-2019.
McDuffie, Erin E., Womack, Caroline C., Fibiger, Dorothy L., Dube, William P., Franchin, Alessandro, Middlebrook, Ann M., Goldberger, Lexie, Lee, Ben H., Thornton, Joel A., Moravek, Alexander, Murphy, Jennifer G., Baasandorj, Munkhbayar, and Brown, Steven S. Fri . "On the contribution of nocturnal heterogeneous reactive nitrogen chemistry to particulate matter formation during wintertime pollution events in Northern Utah". United States. doi:10.5194/acp-19-9287-2019. https://www.osti.gov/servlets/purl/1571482.
@article{osti_1571482,
title = {On the contribution of nocturnal heterogeneous reactive nitrogen chemistry to particulate matter formation during wintertime pollution events in Northern Utah},
author = {McDuffie, Erin E. and Womack, Caroline C. and Fibiger, Dorothy L. and Dube, William P. and Franchin, Alessandro and Middlebrook, Ann M. and Goldberger, Lexie and Lee, Ben H. and Thornton, Joel A. and Moravek, Alexander and Murphy, Jennifer G. and Baasandorj, Munkhbayar and Brown, Steven S.},
abstractNote = {Mountain basins in Northern Utah, including the Salt Lake Valley (SLV), suffer from wintertime air pollution events associated with stagnant atmospheric conditions. During these events, fine particulate matter concentrations (PM2.5) can exceed national ambient air quality standards. Previous studies in the SLV have found that PM2.5 is primarily composed of ammonium nitrate (NH4NO3), formed from the condensation of gas-phase ammonia (NH3) and nitric acid (HNO3).Additional studies in several western basins, including the SLV, have suggested that production of HNO3 from nocturnal heterogeneous N2O5 uptake is the dominant source of NH4NO3 during winter. The rate of this process, however, remains poorly quantified, in part due to limited vertical measurements above the surface, where this chemistry is most active. The 2017 Utah Winter Fine Particulate Study(UWFPS) provided the first aircraft measurements of detailed chemical composition during wintertime pollution events in the SLV. Coupled with ground-based observations, analyses of day- and nighttime research flights confirm that PM2.5 during wintertime pollution events is principally composed of NH4NO3, limited by HNO3. Here, observations and box model analyses assess the contribution of N2O5 uptake to nitrate aerosol during pollution events using the $\mathrm{NO^{-}_{3}}$ production rate, N2O5 heterogeneous uptake coefficient (γ(N2O5)), and production yield of ClNO2 (φ(ClNO2)), which had medians of 1.6 µg m-3 h-1, 0.076,and 0.220, respectively. While fit values of γ(N2O5) maybe biased high by a potential under-measurement in aerosol surface area,other fit quantities are unaffected. Lastly, additional model simulations suggest nocturnal N2O5 uptake produces between 2.4 and 3.9 µg m-3 of nitrate per day when considering the possible effects of dilution. This nocturnal production is sufficient to account for 52 %–85 %of the daily observed surface-level buildup of aerosol nitrate, though accurate quantification is dependent on modeled dilution, mixing processes,and photochemistry.},
doi = {10.5194/acp-19-9287-2019},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 14,
volume = 19,
place = {United States},
year = {2019},
month = {7}
}

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