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Aqueous-Phase Secondary Organic Aerosol and Organosulfate Formation in Atmospheric Aerosols: A Modeling Study
Abstract
We have examined aqueous-phase secondary organic aerosol (SOA) and organosulfate (OS) formation in atmospheric aerosols using a photochemical box model with coupled gas-phase chemistry and detailed aqueous aerosol chemistry. SOA formation in deliquesced ammonium sulfate aerosol is highest under low-NO(x) conditions, with acidic aerosol (pH = 1) and low ambient relative humidity (40%). Under these conditions, with an initial sulfate loading of 4.0 μg m(-3), 0.9 μg m(-3) SOA is predicted after 12 h. Low-NO(x) aqueous-aerosol SOA (aaSOA) and OS formation is dominated by isoprene-derived epoxydiol (IEPOX) pathways; 69% or more of aaSOA is composed of IEPOX, 2-methyltetrol, and 2-methyltetrol sulfate ester. 2-Methyltetrol sulfate ester comprises >99% of OS mass (66 ng m(-3) at 40% RH and pH 1). In urban (high-NO(x)) environments, aaSOA is primarily formed via reversible glyoxal uptake, with 0.12 μg m(-3) formed after 12 h at 80% RH, with 20 μg m(-3) initial sulfate. OS formation under all conditions studied is maximum at low pH and lower relative humidities (<60% RH), i.e., when the aerosol is more concentrated. Therefore, OS species are expected to be good tracer compounds for aqueous aerosol-phase chemistry (vs cloudwater processing).
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Evolution of Organic Aerosols in the Atmosphere
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., et al. (2009) · Science · doi:10.1126/science.1180353 · Cited by 4,167
Cited by
Pöschl, U., & Shiraiwa, M. (2015) · Chemical Reviews · doi:10.1021/cr500487s · Cited by 657
Air Quality and Climate Connections
Fiore, A. M., Naik, V., & Leibensperger, E. M. (2015) · Journal of the Air & Waste Management Association · doi:10.1080/10962247.2015.1040526 · Cited by 537
Compilation of Henry's law constants (version 5.0.0) for water as solvent
Sander, R. (2023) · Atmospheric Chemistry and Physics · doi:10.5194/acp-23-10901-2023 · Cited by 474
Hu, W., Hu, M., Hu, W., Jimenez, J. L., Yuan, B., Chen, W., Wang, M., Wu, Y., Chen, C., Wang, Z., et al. (2016) · Journal of Geophysical Research: Atmospheres · doi:10.1002/2015jd024020 · Cited by 401
Li, Y., Pöschl, U., & Shiraiwa, M. (2016) · Atmospheric Chemistry and Physics · doi:10.5194/acp-16-3327-2016 · Cited by 384
Metadata
- Authors
- McNeill, V. F., Woo, J. L., Kim, D. D., Schwier, A. N., Wannell, N. J., Sumner, A. J., & Barakat, J. M.
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-07-25
- Volume
- 46
- Issue
- 15
- Pages
- 8075-8081
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2034838692
- Cited by
- 230
- References
- 1
- FWCI
- 8.71
- Type
- journal article
- Language
- en
- Open access
- closed
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- McNeill, V. F., Woo, J. L., Kim, D. D., Schwier, A. N., Wannell, N. J., Sumner, A. J., & Barakat, J. M. (2012). Aqueous-Phase Secondary Organic Aerosol and Organosulfate Formation in Atmospheric Aerosols: A Modeling Study. Environmental Science & Technology. https://doi.org/10.1021/es3002986
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Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
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