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.

A sea breeze is a local circulation that occurs in coastal regions from the poles to the equator. The adverse influence of ship emissions on air quality in coastal areas may be aggravated by the onshore flow of sea breeze circulation. However, our knowledge regarding the evolution of ship-emitted pollutants during a specific sea breeze episode is still limited. To address this knowledge gap, this study investigated the evolution of ship emissions during a sea breeze episode that occurred on 29 June, 2014 in Tangshan port in China by employing the WRF/Chem model. NO2, one of the primary pollutants emitted by ships, was selected as the target pollutant for investigation. The results indicate that the ground level NO2 concentration was considerably affected by sea breeze circulation. Although the onset of the sea breeze was delayed until nearly midday due to offshore synoptic winds, ship-emitted NO2 was transported to more than 100 km inland with the penetration of the sea breeze. Further investigation found that the averaged concentration of ship-contributed NO2 during the episode showed an evident downward trend as the distance from the coastline increased. Vertically, the shallow atmospheric boundary layer (ABL) on the sea limited the vertical dispersion of ship emissions, and the pollutant was transported shoreward by the sea breeze within this shallow ABL. The height of the ABLs is lowered in coastal regions due to the cooling effect of sea breezes which brings the cool marine air to the hot land surface. Ship-contributed NO2 was mostly trapped in the shallow ABL; thereby, its concentration increased.

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