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Quantifying the Contributions of Aerosol- and Snow-Produced ClNO2 through Observations and 1D Modeling

  • Daun Jeong
    Daun Jeong
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
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  • Stephen M. McNamara
    Stephen M. McNamara
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
  • Qianjie Chen
    Qianjie Chen
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
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  • Jessica Mirrielees
    Jessica Mirrielees
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
  • Jacinta Edebeli
    Jacinta Edebeli
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
    Paul Scherrer Institut, Villigen 5232, Switzerland
  • Kathryn D. Kulju
    Kathryn D. Kulju
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
  • Siyuan Wang
    Siyuan Wang
    Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, Colorado 80305, United States
    Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado 80309, United States
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  • Laila Hayani
    Laila Hayani
    Applied Physics Program, University of Michigan, Ann Arbor, Michigan 48109, United States
    More by Laila Hayani
  • Rachel M. Kirpes
    Rachel M. Kirpes
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
  • Nurun Nahar Lata
    Nurun Nahar Lata
    Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
  • Swarup China
    Swarup China
    Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
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  • Jose D. Fuentes
    Jose D. Fuentes
    Department of Meteorology and Atmospheric Science, The Pennsylvania State University, University Park, Pennsylvania 16802 United States
  • , and 
  • Kerri A. Pratt*
    Kerri A. Pratt
    Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States
    Department of Earth and Environmental Sciences, University of Michigan, Ann Arbor, Michigan 48109, United States
    *Email: [email protected]; tel: (734) 763-2871.
Cite this: ACS Earth Space Chem. 2023, 7, 12, 2548–2561
Publication Date (Web):December 4, 2023
https://doi.org/10.1021/acsearthspacechem.3c00237
Copyright © 2023 American Chemical Society

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    Abstract

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    Nitryl chloride (ClNO2) is a radical reservoir that forms and accumulates in the nocturnal atmospheric boundary layer influenced by combustion emissions and chloride (e.g., sea salt and road salt). Upon sunrise, ClNO2 rapidly photolyzes to generate highly reactive chlorine radicals (Cl) that affect the air quality by generating secondary air pollutants. Recent studies have shown road salt aerosols and saline snowpack to be sources of ClNO2 in the wintertime urban environment; however, the quantitative contributions of each chloride source are not known. In this study, we examine the vertically resolved contributions of aerosol particles and saline snowpack as sources of ClNO2 by using an observationally constrained snow–atmosphere coupled one-dimensional model applied to wintertime Kalamazoo, Michigan, U.S. Model simulations show that ClNO2 emitted from urban snowpack can be vertically transported throughout the entire atmospheric boundary layer and can be a significant source of ClNO2, contributing up to ∼60% of the ClNO2 budget near the surface. Modeled snowpack ClNO2 emission rates were 6 (±7) times higher than the observationally derived emission rates, suggesting that not all snow chloride is available for reaction. ClNO2 production from both aerosol particles and snow emissions are required to best simulate the observed surface-level ClNO2. Using the traditional bulk parameterization for ClNO2 produced from particles significantly overestimated ClNO2 due to the assumption of having equivalent dinitrogen pentoxide (N2O5) uptake and chloride availability for the entire particle population. In comparison, the chemically resolved surface area-based parameterization slightly underestimated the observations and had uncertainties deriving from ClNO2 production from residential wood burning particles.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsearthspacechem.3c00237.

    • Further details on CIMS measurements (S1), 1D model setup (S2), turbulent transport calculations in model (S3), heterogeneous reactions on aerosols and snowpack (S4), CCSEM-EDX analysis of particles (S5), and ClNO2 model simulations in residual layer (S6). Additional model constraints (Table S1), snow parameter inputs in the model (Table S2), and N2O5 uptakes and ClNO2 yields of different particle (Table S3). Observed HCl (Figure S1); parameters used in calculating the N2O5 uptake and ClNO2 yield (Figure S2); particle number concentration and total surface area (Figure S3); size distributions of particles (Figure S4); SEM images and EDX spectra of particles (Figure S5); size distribution of particles from CCSEM-EDX (Figure S6); snow N2O5 uptake and ClNO2 yield (Figure S7); diel friction velocity and eddy diffusivity (Figure S8); 1D model schematic (Figure S9); vertical absolute humidity, potential temperature, and eddy diffusivity (Figure S10); estimated boundary layer height and eddy diffusivity (Figure S11); and modeled NO2 (Figure S12) (PDF)

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