The role of coarse aerosol particles as a sink of HNO3 in wintertime pollution events in the Salt Lake Valley
(2021) In Atmospheric Chemistry and Physics 21(10). p.8111-8126- Abstract
Wintertime ammonium nitrate (NH4NO3) pollution events burden urban mountain basins around the globe. In the Salt Lake Valley of Utah in the United States, such pollution events are often driven by the formation of persistent cold-air pools (PCAPs) that trap emissions near the surface for several consecutive days. As a result, secondary pollutants including fine particulate matter less than 2.5 um in diameter (PM2:5), largely in the form of NH4NO3, build up during these events and lead to severe haze. As part of an extensive measurement campaign to understand the chemical processes underlying PM2:5 formation, the 2017 Utah Winter Fine Particulate Study, water-soluble trace gases and PM2:5 constituents were continuously monitored using... (More)
Wintertime ammonium nitrate (NH4NO3) pollution events burden urban mountain basins around the globe. In the Salt Lake Valley of Utah in the United States, such pollution events are often driven by the formation of persistent cold-air pools (PCAPs) that trap emissions near the surface for several consecutive days. As a result, secondary pollutants including fine particulate matter less than 2.5 um in diameter (PM2:5), largely in the form of NH4NO3, build up during these events and lead to severe haze. As part of an extensive measurement campaign to understand the chemical processes underlying PM2:5 formation, the 2017 Utah Winter Fine Particulate Study, water-soluble trace gases and PM2:5 constituents were continuously monitored using the ambient ion monitoring ion chromatograph (AIM-IC) system at the University of Utah campus. Gas-phase NH3, HNO3, HCl, and SO2 along with particulate NHC 4 , NaC, KC, Mg2C, Ca2C, NO3 , Cl, and SO2 4 were measured from 21 January to 21 February 2017. During the two PCAP events captured, the fine particulate matter was dominated by secondary NH4NO3. The comparison of total nitrate (HNO3 CPM2:5 NO3 ) and total NHx (NH3 CPM2:5 NHC 4 ) showed NHx was in excess during both pollution events. However, chemical composition analysis of the snowpack during the first PCAP event revealed that the total concentration of deposited NO3 was nearly 3 times greater than that of deposited NHC 4 . Daily snow composition measurements showed a strong correlation between NO3 and Ca2C in the snowpack. The presence of non-volatile salts (NaC, Ca2C, and Mg2C), which are frequently associated with coarse-mode dust, was also detected in PM2:5 by the AIM-IC during the two PCAP events, accounting for roughly 5% of total mass loading. The presence of a significant particle mass and surface area in the coarse mode during the first PCAP event was indicated by size-resolved particle measurements from an aerodynamic particle sizer. Taken together, these observations imply that atmospheric measurements of the gas-phase and fine-mode particle nitrate may not represent the total burden of nitrate in the atmosphere, implying a potentially significant role for uptake by coarse-mode dust. Using the NO3 :NHC 4 ratio observed in the snowpack to estimate the proportion of atmospheric nitrate present in the coarse mode, we estimate that the amount of secondary NH4NO3 could double in the absence of the coarse-mode sink. The underestimation of total nitrate indicates an incomplete account of the total oxidant production during PCAP events. The ability of coarse particles to permanently remove HNO3 and influence PM2:5 formation is discussed using information about particle composition and size distribution.
(Less)
- author
- organization
- publishing date
- 2021-05
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Atmospheric Chemistry and Physics
- volume
- 21
- issue
- 10
- pages
- 16 pages
- publisher
- Copernicus GmbH
- external identifiers
-
- scopus:85106951871
- ISSN
- 1680-7316
- DOI
- 10.5194/acp-21-8111-2021
- language
- English
- LU publication?
- yes
- id
- c06b40d5-e55c-499b-b573-985cbf253eeb
- date added to LUP
- 2022-01-04 10:52:58
- date last changed
- 2023-02-21 09:59:30
@article{c06b40d5-e55c-499b-b573-985cbf253eeb,
abstract = {{<p>Wintertime ammonium nitrate (NH4NO3) pollution events burden urban mountain basins around the globe. In the Salt Lake Valley of Utah in the United States, such pollution events are often driven by the formation of persistent cold-air pools (PCAPs) that trap emissions near the surface for several consecutive days. As a result, secondary pollutants including fine particulate matter less than 2.5 um in diameter (PM2:5), largely in the form of NH4NO3, build up during these events and lead to severe haze. As part of an extensive measurement campaign to understand the chemical processes underlying PM2:5 formation, the 2017 Utah Winter Fine Particulate Study, water-soluble trace gases and PM2:5 constituents were continuously monitored using the ambient ion monitoring ion chromatograph (AIM-IC) system at the University of Utah campus. Gas-phase NH3, HNO3, HCl, and SO2 along with particulate NHC 4 , NaC, KC, Mg2C, Ca2C, NO3 , Cl, and SO2 4 were measured from 21 January to 21 February 2017. During the two PCAP events captured, the fine particulate matter was dominated by secondary NH4NO3. The comparison of total nitrate (HNO3 CPM2:5 NO3 ) and total NHx (NH3 CPM2:5 NHC 4 ) showed NHx was in excess during both pollution events. However, chemical composition analysis of the snowpack during the first PCAP event revealed that the total concentration of deposited NO3 was nearly 3 times greater than that of deposited NHC 4 . Daily snow composition measurements showed a strong correlation between NO3 and Ca2C in the snowpack. The presence of non-volatile salts (NaC, Ca2C, and Mg2C), which are frequently associated with coarse-mode dust, was also detected in PM2:5 by the AIM-IC during the two PCAP events, accounting for roughly 5% of total mass loading. The presence of a significant particle mass and surface area in the coarse mode during the first PCAP event was indicated by size-resolved particle measurements from an aerodynamic particle sizer. Taken together, these observations imply that atmospheric measurements of the gas-phase and fine-mode particle nitrate may not represent the total burden of nitrate in the atmosphere, implying a potentially significant role for uptake by coarse-mode dust. Using the NO3 :NHC 4 ratio observed in the snowpack to estimate the proportion of atmospheric nitrate present in the coarse mode, we estimate that the amount of secondary NH4NO3 could double in the absence of the coarse-mode sink. The underestimation of total nitrate indicates an incomplete account of the total oxidant production during PCAP events. The ability of coarse particles to permanently remove HNO3 and influence PM2:5 formation is discussed using information about particle composition and size distribution.</p>}},
author = {{Hrdina, Amy and Murphy, Jennifer G. and Hallar, Anna Gannet and Lin, John C. and Moravek, Alexander and Bares, Ryan and Petersen, Ross C. and Franchin, Alessandro and Middlebrook, Ann M. and Goldberger, Lexie and Lee, Ben H. and Baasandorj, Munkh and Brown, Steven S.}},
issn = {{1680-7316}},
language = {{eng}},
number = {{10}},
pages = {{8111--8126}},
publisher = {{Copernicus GmbH}},
series = {{Atmospheric Chemistry and Physics}},
title = {{The role of coarse aerosol particles as a sink of HNO3 in wintertime pollution events in the Salt Lake Valley}},
url = {{http://dx.doi.org/10.5194/acp-21-8111-2021}},
doi = {{10.5194/acp-21-8111-2021}},
volume = {{21}},
year = {{2021}},
}