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Heterogeneous sulfate aerosol formation mechanisms during wintertime Chinese haze events: air quality model assessment using observations of sulfate oxygen isotopes in Beijing
Ist Teil von
Atmospheric chemistry and physics, 2019-05, Vol.19 (9), p.6107-6123
Ort / Verlag
Katlenburg-Lindau: Copernicus GmbH
Erscheinungsjahr
2019
Link zum Volltext
Quelle
EZB Free E-Journals
Beschreibungen/Notizen
Air quality models have not been able to reproduce the magnitude of the
observed concentrations of fine particulate matter (PM2.5) during
wintertime Chinese haze events. The discrepancy has been at least partly
attributed to low biases in modeled sulfate production rates, due to the lack
of heterogeneous sulfate production on aerosols
in the models. In this study, we explicitly implement four heterogeneous sulfate formation
mechanisms into a regional chemical transport model, in addition to
gas-phase and in-cloud sulfate production. We compare the model results with
observations of sulfate concentrations and oxygen isotopes, Δ17O(SO42-), in the winter of 2014–2015, the latter of which
is highly sensitive to the relative importance of different sulfate
production mechanisms. Model results suggest that heterogeneous sulfate
production on aerosols accounts for about 20 % of sulfate production in
clean and polluted conditions, partially reducing the modeled low bias in
sulfate concentrations. Model sensitivity studies in comparison with the
Δ17O(SO42-) observations suggest that heterogeneous
sulfate formation is dominated by transition metal ion-catalyzed oxidation of SO2.