Thermodynamic Modeling Suggests Declines in Water Uptake and Acidity of Inorganic Aerosols in Beijing Winter Haze Events during 2014/2015-2018/2019

During recent years, aggressive air pollution mitigation measures in northern China have resulted in considerable changes in gas and aerosol chemical composition. But it is unclear whether aerosol water content and acidity respond to these changes. The two parameters have been shown to affect heterogeneous production of winter haze aerosols. Here, we performed thermodynamic equilibrium modeling using chemical and meteorological data observed in urban Beijing for four recent winter seasons and quantified the changes in the mass growth factor and pH of inorganic aerosols. We focused on high relative humidity (>60%) conditions when submicron particles have been shown to be in the liquid state. From 2014/2015 to 2018/2019, the modeled mass growth factor decreased by about 9%-17% due to changes in aerosol compositions (more nitrate and less sulfate and chloride), and the modeled pH increased by about 0.3-0.4 unit mainly due to rising ammonia. A buffer equation is derived from semivolatile ammonia partitioning, which helps understand the sensitivity of pH to meteorological and chemical variables. The findings provide implications for evaluating the potential chemical feedback in secondary aerosol production and the effectiveness of ammonia control as a measure to alleviate winter haze.