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

Jeong, Daun; McNamara, Stephen M.; Chen, Qianjie; Mirrielees, Jessica; Edebeli, Jacinta; Kulju, Kathryn D.; Wang, Siyuan; Hayani, Laila; Kirpes, Rachel M.; Lata, Nurun Nahar; China, Swarup; Fuentes, Jose D.; Pratt, Kerri A.

doi:10.1021/acsearthspacechem.3c00237

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

Journal Article · Mon Dec 04 00:00:00 EST 2023 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.3c00237· OSTI ID:2337662

Jeong, Daun ^[1]; McNamara, Stephen M. ^[2]; Chen, Qianjie ^[3]; Mirrielees, Jessica ^[2]; Edebeli, Jacinta ^[4]; Kulju, Kathryn D. ^[2]; ^[5]; Hayani, Laila ^[2]; ^[2]; Lata, Nurun Nahar ^[6]; ^[6]; Fuentes, Jose D. ^[7]; ^[2]

Univ. of Michigan, Ann Arbor, MI (United States); National Center for Atmospheric Research (NCAR), Boulder, CO (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Univ. of Michigan, Ann Arbor, MI (United States); Hong Kong Polytechnic Univ. (Hong Kong)
Univ. of Michigan, Ann Arbor, MI (United States); Paul Scherrer Inst. (PSI), Villigen (Switzerland); Zurich University of Applied Sciences (ZHAW) (Switzerland)
National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States); Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences (CIRES)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)
Pennsylvania State Univ., University Park, PA (United States)

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. Here, 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.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Oceanic and Atmospheric Administration (NOAA); National Science Foundation (NSF); USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2337662

Report Number(s):: PNNL-SA--191621

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 12 Vol. 7; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Fast heterogeneous N ₂ O ₅ uptake and ClNO ₂ production in power plant and industrial plumes observed in the nocturnal residual layer over the North China Plain Wang, Zhe; Wang, Weihao; Tham, Yee Jun Atmospheric Chemistry and Physics, Vol. 17, Issue 20 https://doi.org/10.5194/acp-17-12361-2017	journal	January 2017
A new mechanism for atmospheric mercury redox chemistry: implications for the global mercury budget Horowitz, Hannah M.; Jacob, Daniel J.; Zhang, Yanxu Atmospheric Chemistry and Physics, Vol. 17, Issue 10 https://doi.org/10.5194/acp-17-6353-2017	journal	January 2017
Heterogeneous N ₂ O ₅ uptake coefficient and production yield of ClNO ₂ in polluted northern China: roles of aerosol water content and chemical composition Tham, Yee Jun; Wang, Zhe; Li, Qinyi Atmospheric Chemistry and Physics, Vol. 18, Issue 17 https://doi.org/10.5194/acp-18-13155-2018	journal	January 2018
Low levels of nitryl chloride at ground level: nocturnal nitrogen oxides in the Lower Fraser Valley of British Columbia Osthoff, Hans D.; Odame-Ankrah, Charles A.; Taha, Youssef M. Atmospheric Chemistry and Physics, Vol. 18, Issue 9 https://doi.org/10.5194/acp-18-6293-2018	journal	May 2018
Integration of airborne and ground observations of nitryl chloride in the Seoul metropolitan area and the implications on regional oxidation capacity during KORUS-AQ 2016 Jeong, Daun; Seco, Roger; Gu, Dasa Atmospheric Chemistry and Physics, Vol. 19, Issue 19 https://doi.org/10.5194/acp-19-12779-2019	journal	January 2019
The role of chlorine in global tropospheric chemistry Wang, Xuan; Jacob, Daniel J.; Eastham, Sebastian D. Atmospheric Chemistry and Physics, Vol. 19, Issue 6 https://doi.org/10.5194/acp-19-3981-2019	journal	January 2019
pH-dependent production of molecular chlorine, bromine, and iodine from frozen saline surfaces Halfacre, John W.; Shepson, Paul B.; Pratt, Kerri A. Atmospheric Chemistry and Physics, Vol. 19, Issue 7 https://doi.org/10.5194/acp-19-4917-2019	journal	January 2019
Urban inland wintertime N₂O₅ and ClNO₂ influenced by snow-covered ground, air turbulence, and precipitation Kulju, Kathryn D.; McNamara, Stephen M.; Chen, Qianjie Atmospheric Chemistry and Physics, Vol. 22, Issue 4 https://doi.org/10.5194/acp-22-2553-2022	journal	February 2022
The origin of sea salt in snow on Arctic sea ice and in coastal regions Domine, F.; Sparapani, R.; Ianniello, A. Atmospheric Chemistry and Physics, Vol. 4, Issue 9/10 https://doi.org/10.5194/acp-4-2259-2004	journal	January 2004
The effect of varying levels of surfactant on the reactive uptake of N₂O₅ to aqueous aerosol McNeill, V. F.; Patterson, J.; Wolfe, G. M. Atmospheric Chemistry and Physics, Vol. 6, Issue 6 https://doi.org/10.5194/acp-6-1635-2006	journal	January 2006
An overview of snow photochemistry: evidence, mechanisms and impacts Grannas, A. M.; Jones, A. E.; Dibb, J. Atmospheric Chemistry and Physics, Vol. 7, Issue 16 https://doi.org/10.5194/acp-7-4329-2007	journal	January 2007
Snow physics as relevant to snow photochemistry Domine, F.; Albert, M.; Huthwelker, T. Atmospheric Chemistry and Physics, Vol. 8, Issue 2 https://doi.org/10.5194/acp-8-171-2008	journal	January 2008
Parameterization of N ₂ O ₅ reaction probabilities on the surface of particles containing ammonium, sulfate, and nitrate Davis, J. M.; Bhave, P. V.; Foley, K. M. Atmospheric Chemistry and Physics, Vol. 8, Issue 17 https://doi.org/10.5194/acp-8-5295-2008	journal	January 2008
The role of ice in N₂O₅ heterogeneous hydrolysis at high latitudes Apodaca, R. L.; Huff, D. M.; Simpson, W. R. Atmospheric Chemistry and Physics, Vol. 8, Issue 24 https://doi.org/10.5194/acp-8-7451-2008	journal	December 2008
Toward a general parameterization of N ₂ O ₅ reactivity on aqueous particles: the competing effects of particle liquid water, nitrate and chloride Bertram, T. H.; Thornton, J. A. Atmospheric Chemistry and Physics, Vol. 9, Issue 21 https://doi.org/10.5194/acp-9-8351-2009	journal	January 2009
Chlorine activation by N ₂ O ₅ : simultaneous, in situ detection of ClNO ₂ and N ₂ O ₅ by chemical ionization mass spectrometry Kercher, J. P.; Riedel, T. P.; Thornton, J. A. Atmospheric Measurement Techniques, Vol. 2, Issue 1 https://doi.org/10.5194/amt-2-193-2009	journal	January 2009

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