Atmospheric sulfate aerosol formation enhanced by interfacial anions
Creators
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1.
East China Normal University
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2.
Guangdong University of Technology
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3.
Chinese Research Academy of Environmental Sciences
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4.
Harbin Institute of Technology
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5.
Stanford University
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6.
California Institute of Technology
Contributors
Editor:
Abstract
Heterogeneous oxidation of SO2 by NO2 on aerosols has recently been found to be one of the major formation pathways of sulfate in the polluted troposphere, but the chemical mechanisms and kinetics remain uncertain. By combining lab experiments, theoretical chemistry calculations, and field measurements, here we show that the SO2 oxidation by NO2 is critically dependent on anions at the air–aerosol aqueous interface. The reaction rate of NO2 with HSO⁻₃ (1.1 × 108–1.6 × 109 M−1 s−1) is more than four orders of magnitude larger than the traditionally held value for the bulk phase due to the abundant occurrence of chloride, nitrate, and carboxylic anions at the air–aqueous interface, which remarkably accelerates sulfate formation during China haze periods by enhancing the uptake of NO2 through interfacial electrostatic attraction. Atmospheric models not accounting for this aerosol interfacial process likely produce major misrepresentations of tropospheric sulfate aerosols under polluted conditions.
Copyright and License
Funding
This work was financially supported by the National Natural Science Foundation of China (nos. 42130704 and U23A2030) and the National Key Research and Development Program of China (2023YFC3706302).
Contributions
G.W. conceived and designed the research. S.Z., X.X., S.G., and G.W. conducted the lab chamber experiments. S.Z., S.G., and G.W. analyzed the chamber experiment data. T.Z., H.S., and G.W. performed the theoretical chemistry calculation. J.G., Y.R., and H.L. collected the field samples. C.W. and G.W. analyzed the field observation data. G.W. wrote the paper. Other authors contributed to this work with useful discussions and comments.
G.W. and S.Z. contributed equally to this work.
Data Availability
The chamber experiments and field observation data are available at https://doi.org/10.5281/zenodo.14898280, while all other data can be found at the Supplementary material.
Supplemental Material
Additional Information
This manuscript was posted as a preprint at: https://doi.org/10.21203/rs.3.rs-2230064/v1.
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Additional details
Additional titles
- Alternative title
- Atmospheric sulfate formation from SO₂ oxidation by NO₂ is enhanced by charges at the air-aqueous interface
Identifiers
- PMCID
- PMC11880798
Related works
- Describes
- Journal Article: PMC11880798 (PMCID)
- Is new version of
- Discussion Paper: 10.21203/rs.3.rs-2230064/v1 (DOI)
- Is supplemented by
- Dataset: 10.5281/zenodo.14898280 (DOI)
Funding
- National Natural Science Foundation of China
- 42130704
- National Natural Science Foundation of China
- U23A2030
- National Key R&D Plan, Ministry of Science and Technology of China
- 2023YFC3706302
Dates
- Accepted
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2025-02-10
- Available
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2025-02-24Published
- Available
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2025-03-05Corrected and typeset