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Related Experiment Videos

Electron-triggered chemistry in HNO3/H2O complexes.

Jozef Lengyel1, Milan Ončák, Juraj Fedor

  • 1J. Heyrovský Institute of Physical Chemistry v.v.i., Czech Academy of Sciences, Dolejškova 3, 18223 Prague, Czech Republic. michal.farnik@jh-inst.cas.cz.

Physical Chemistry Chemical Physics : PCCP
|April 12, 2017
PubMed
Summary

Researchers studied nitric acid-water clusters in polar stratospheric clouds. Electron attachment reactions unexpectedly formed nitrate anions, revealing new atmospheric sources of OH and HONO molecules.

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Area of Science:

  • Atmospheric Chemistry
  • Physical Chemistry
  • Spectroscopy

Background:

  • Polar stratospheric clouds (PSCs) are crucial for stratospheric chemistry, primarily composed of nitric acid (HNO3) ice particles.
  • Understanding the behavior of HNO3-water clusters is key to elucidating PSC formation and chemical processes.
  • Previous studies on electron attachment to HNO3 primarily focused on the gas phase, yielding different ionic products.

Purpose of the Study:

  • To investigate the formation and reactions of mixed nitric acid-water clusters (HNO3)m(H2O)n under simulated stratospheric conditions.
  • To identify the primary ionic species and reaction pathways resulting from electron attachment to these clusters.
  • To explore potential new sources of atmospherically relevant molecules generated through these reactions.

Main Methods:

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  • Laboratory experiments using a molecular beam setup combined with electron attachment (0-14 eV) and mass spectrometry.
  • Density Functional Theory (DFT) calculations to interpret experimental observations and reaction mechanisms.
  • Analysis of intracluster ion-molecule reactions following electron attachment.

Main Results:

  • Electron attachment to mixed nitric acid-water clusters predominantly forms the nitrate anion (NO3-), contrary to gas-phase HNO3 electron attachment which yields nitrite (NO2-).
  • Nitrate-containing clusters are terminal products formed via at least three distinct reaction pathways.
  • Complex reaction cascades initiated by electron attachment generate previously unrecognized atmospheric sources of hydroxyl (OH) and nitrous acid (HONO).

Conclusions:

  • The central role of the nitrate anion (NO3-) in electron-induced reactions of HNO3-water clusters is a significant finding.
  • These reactions represent a novel source of OH and HONO, impacting stratospheric chemistry.
  • The study highlights the importance of considering cluster effects in atmospheric chemical processes involving nitric acid.