TY - JOUR
T1 - On the contribution of nocturnal heterogeneous reactive nitrogen chemistry to particulate matter formation during wintertime pollution events in Northern Utah
AU - McDuffie, Erin E.
AU - Womack, Caroline C.
AU - Fibiger, Dorothy L.
AU - Dube, William P.
AU - Franchin, Alessandro
AU - Middlebrook, Ann M.
AU - Goldberger, Lexie
AU - Lee, Ben H.
AU - Thornton, Joel A.
AU - Moravek, Alexander
AU - Murphy, Jennifer G.
AU - Baasandorj, Munkhbayar
AU - Brown, Steven S.
N1 - Publisher Copyright:
© 2019 Author(s).
PY - 2019/7/19
Y1 - 2019/7/19
N2 - 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 NO-3 production rate, N2O5 heterogeneous uptake coefficient (?.N2O5/), and production yield of ClNO2 ('.ClNO2/), which had medians of 1.6 μg m-3 h-1, 0.076, and 0.220, respectively. While fit values of.N2O5/may be 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.
AB - 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 NO-3 production rate, N2O5 heterogeneous uptake coefficient (?.N2O5/), and production yield of ClNO2 ('.ClNO2/), which had medians of 1.6 μg m-3 h-1, 0.076, and 0.220, respectively. While fit values of.N2O5/may be 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.
UR - https://www.scopus.com/pages/publications/85069760612
U2 - 10.5194/acp-19-9287-2019
DO - 10.5194/acp-19-9287-2019
M3 - Article
AN - SCOPUS:85069760612
SN - 1680-7316
VL - 19
SP - 9287
EP - 9308
JO - Atmospheric Chemistry and Physics
JF - Atmospheric Chemistry and Physics
IS - 14
ER -