Mechanism of nitrate formation in atmospheric haze particlesre

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Abstract

The paper considers data on winter monitoring of the ionic composition of aerosol particles and small gas components in the surface atmosphere of Antwerp and Beijing. According to the results of their comparison, it is shown that the rapid accumulation of NO3- over Beijing in haze particles is triggered by a liquid-phase catalytic reaction of sulfate formation involving Mn/Fe ions, which proceeds in a fast degenerate branched mode. The cycle of these transformations is accompanied by the associated production of nitrate radicals in the particles. Their release into the gas phase leads to an increase in the concentration of N2O5 molecules, and a rapid accumulation of nitrates. The coupling of the catalytic (petrochemical) conversion of sulfur dioxide into sulfates and the nitrate production process over Beijing thus plays a crucial role in the formation of the mineral composition of haze particles in the atmosphere.

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G. B. Pronchev

Semenov Federal Research Center for Chemical Physics Russian Academy of Sciences

Author for correspondence.
Email: pronchev@rambler.ru
Russian Federation, Moscow

A. N. Yermakov

Semenov Federal Research Center for Chemical Physics Russian Academy of Sciences

Email: pronchev@rambler.ru
Russian Federation, Moscow

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2. Fig. 1. Dependence of the ratio of mass concentrations (μmol m-3) of nitrates and sulfates in aerosol particles over Antwerp (gray circles) and in haze particles over Beijing (light circles) on the relative air humidity. The inset shows the change in the ratio of nitrates and nitric acid vapors over Antwerp depending on the moisture content of the particles.

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3. Fig. 2. Correspondence between calculated ([NO-3(aer)]calc) and measured ([NO-3(aer)]meas) nitrate concentrations (gray dots) in aerosol particles over Antwerp (19–21 December 2003) [21]. Light dots – [NO-3(aer)]meas calculations using the nitric acid vapour concentration averaged over all episodes. Solid line – data correspondence with a correlation coefficient equal to one.

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4. Fig. 3. Dependence of mass concentrations of nitrates (main field of the figure) and sulfates (inset) in haze particles over Beijing on their moisture content.

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5. Fig. 4. Effect of sulfate content on the volumetric moisture content of haze particles (Beijing, December 2016) – data from monitoring and thermodynamic calculations [22]. Black circles in open circles – sample of episodes with pH < 3.5, black triangles in open circles – sample with pH > 4.3 (see text).

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