modeling atmospheric mineral aerosol chemistry to predict heterogeneous photooxidation of so2
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2017
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Abstract
The photocatalytic ability of airborne mineral dust particles is
known to heterogeneously promote SO2 oxidation, but prediction of this
phenomenon is not fully taken into account by current models. In this study,
the Atmospheric Mineral Aerosol Reaction (AMAR) model was developed to
capture the influence of air-suspended mineral dust particles on sulfate
formation in various environments. In the model, SO2 oxidation proceeds
in three phases including the gas phase, the inorganic-salted aqueous phase
(non-dust phase), and the dust phase. Dust chemistry is described as the
absorption–desorption kinetics of SO2 and NOx (partitioning
between the gas phase and the multilayer coated dust). The reaction of
absorbed SO2 on dust particles occurs via two major paths:
autoxidation of SO2 in open air and photocatalytic mechanisms under UV
light. The kinetic mechanism of autoxidation was first leveraged using
controlled indoor chamber data in the presence of Arizona Test Dust (ATD)
particles without UV light, and then extended to photochemistry. With UV
light, SO2 photooxidation was promoted by surface oxidants (OH radicals)
that are generated via the photocatalysis of semiconducting metal oxides
(electron–hole theory) of ATD particles. This photocatalytic rate constant
was derived from the integration of the combinational product of the dust
absorbance spectrum and wave-dependent actinic flux for the full range of
wavelengths of the light source. The predicted concentrations of sulfate and
nitrate using the AMAR model agreed well with outdoor chamber data that were
produced under natural sunlight. For seven consecutive hours of
photooxidation of SO2 in an outdoor chamber, dust chemistry at the low
NOx level was attributed to 55 % of total sulfate (56 ppb SO2,
290 µg m−3 ATD, and NOx less than 5 ppb). At high
NOx ( > 50 ppb of NOx with low hydrocarbons), sulfate formation
was also greatly promoted by dust chemistry, but it was suppressed by the
competition between NO2 and SO2, which both consume the dust-surface
oxidants (OH radicals or ozone).
| Reference Key |
yu2017atmosphericmodeling
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|---|---|
| Authors | ;Z. Yu;M. Jang;J. Park |
| Journal | Journal of agricultural and food chemistry |
| Year | 2017 |
| DOI |
10.5194/acp-17-10001-2017
|
| URL | |
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