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Microdroplet Surface Drives and Accelerates Proton-Controlled, Size-Dependent Nitrate Photolysis.

Xiaowu Zhang1, Qishen Huang1, Yu-Xin Liu1

  • 1School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China.

Journal of the American Chemical Society
|June 2, 2025
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Summary

Particulate nitrate photolysis rates vary due to droplet size and pH. This study reveals surface-driven, size-dependent photolysis in microdroplets, explaining atmospheric variations in reactive nitrogen regeneration.

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Area of Science:

  • Atmospheric Chemistry
  • Environmental Science
  • Physical Chemistry

Background:

  • Particulate nitrate photolysis releases reactive oxidized nitrogen species (HONO and NOx), impacting air quality and climate.
  • Existing data on nitrate photolysis rates show significant variability, with unclear roles for protons and the air-water interface in aerosols.
  • Understanding these processes is crucial for accurate atmospheric modeling.

Purpose of the Study:

  • To investigate the influence of pH and droplet size on nitrate photolysis rate coefficients in microdroplets.
  • To elucidate the roles of protons and the air-water interface in nitrate photolysis within deliquesced aerosols.
  • To resolve discrepancies in reported nitrate photolysis rates and explain atmospheric variability.

Main Methods:

  • Utilized confocal Raman spectroscopy and aerosol optical tweezer techniques.
  • Measured nitrate photolysis rate coefficients (j) in microdroplets across a range of pH (3.2-7.4) and radii (3.7 μm to 6.0 mm).
  • Analyzed the dependence of photolysis rates on pH and droplet size, identifying tipping points.

Main Results:

  • Nitrate photolysis rate coefficients ranged from 5.28 × 10⁻⁸ to 9.07 × 10⁻⁶ s⁻¹.
  • Photolysis rates were pH-independent below pH 6.5 and decreased with increasing pH above 6.5.
  • A tipping-point radius (r* = 706 μm) was identified, below which photolysis scaled inversely with radius, indicating surface dominance.

Conclusions:

  • Nitrate photolysis predominantly occurs at the air-water interface in microdroplets.
  • The identified size-dependent photolysis mechanism explains the observed variations in atmospheric particulate nitrate photolysis rates.
  • Findings are critical for improving atmospheric models of nitrogen cycling and air quality.