There is a large gap between the simulated and observed sulfate concentrations during winter haze events in North China. Although multiphase sulfate formation mechanisms have been proposed, they have not been evaluated using chemical transport models. In this study, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) was used to apportion sulfate formation. It was found that Mncatalyzed oxidation on aerosol surfaces was the dominant sulfate formation pathway, accounting for 92.3 ± 3.5% of the sulfate formation during haze events. Gas-phase oxidation contributed 3.1 ± 0.5% to the sulfate formation due to the low OH levels. The H 2 O 2 oxidation in aerosol water accounted for 4.2 ± 3.6% of the sulfate formation, caused by the rapid consumption of H 2 O 2 . The contributions of O 3 , NO 2 oxidation, and transition metal ion-catalyzed reactions in aerosol water could be negligible owing to the low aerosol water content, low pH, and high ionic strength. The contributions from in-cloud reactions were negligible due to the barrier provided by stable stratification during winter haze events.
Abstract. Satellite observations show a global maximum in ammonia
(NH3) over the Indo-Gangetic Plain (IGP), with a peak from June to
August. However, it has never been explained explicitly. In this study, we
investigated the causes of high NH3 loading over the IGP during the pre-monsoon and monsoon seasons using WRF-Chem (Weather Research and
Forecasting model coupled to chemistry). The IGP has relatively high NH3 emission fluxes (0.4 t km−2 month−1) due to intensive
agricultural activities and high air temperature from June to August.
Additionally, low sulfur dioxide (SO2) and nitrogen oxides (NOx) emissions and high air temperature limit the gas-to-particle conversion of
NH3, particularly for ammonium nitrate formation. Moreover, the barrier
effects of the Himalayas in combination with the surface convergence weaken
the horizontal diffusion of NH3. The high NH3 loading over the IGP
mainly results from the low gas-to-particle partitioning of NH3 caused
by low SO2 and NOx emissions. It contrasts to those in the North
China Plain, where high SO2 and NOx emissions promote the
conversion of gaseous NH3 into particulate ammonium.
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