Abstract
How tiny aqueous aerosol droplets significantly accelerate the atmospheric multiphase reaction remains an open question. Here, we show both experimental and theoretical evidence that the strong electric field at the air/water interface of aerosol particles can be an important driving force contributing to the fast oxidation of SO2-forming sulfate. We mapped out the spatial surface enrichment of sulfate in nitrate microdroplets using 2D laser confocal Raman microscopy and molecular dynamics (MD) simulations. Strong electric fields up to ∼1 × 108 V cm−1 are determined for the aerosol air/water interface, thus highlighting an important role of electrostatic force in atmospherically relevant chemistry. The detailed SO2 oxidation reaction mechanism triggered by the electric field was further elucidated by density functional theory (DFT) calculations. Overall, this work provides a new perspective, we think, about chemical reactions in the atmosphere and may potentially change the framework of current knowledge concerning the atmospheric chemical process.
Original language | English (US) |
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Pages (from-to) | 330-351 |
Number of pages | 22 |
Journal | Chem |
Volume | 10 |
Issue number | 1 |
DOIs | |
State | Published - Jan 11 2024 |
Bibliographical note
Publisher Copyright:© 2023 Elsevier Inc.
Keywords
- air/water interface
- electric field
- multiphase oxidation
- nitrate photolysis
- SDG13: Climate action
- SDG3: Good health and well-being
- SO oxidation
- sulfate production
ASJC Scopus subject areas
- General Chemistry
- Biochemistry
- Environmental Chemistry
- General Chemical Engineering
- Biochemistry, medical
- Materials Chemistry