Rapid transition in winter aerosol composition in Beijing from 2014 to 2017: response to clean air actions

The clean air actions implemented by the Chinese government in 2013 have led to significantly improved air quality in Beijing. In this work, we combined the in situ measurements of the chemical components of submicron particles (PM1) in Beijing during the winters of 2014 and 2017 and a regional chemical transport model to investigate the impact of clean air actions on aerosol chemistry and quantify the relative contributions of anthropogenic emissions, meteorological conditions, and regional transport to the changes in aerosol chemical composition from 2014 to 2017. We found that the average PM1 concentration in winter in Beijing decreased by 49.5 % from 2014 to 2017 (from 66.2 to 33.4 mu g m(-3)). Sulfate exhibited a much larger decline than nitrate and ammonium, which led to a rapid transition from sulfate-driven to nitrate-driven aerosol pollution during the wintertime. Organic aerosol (OA), especially coal combustion OA, and black carbon also showed large decreasing rates, indicating the effective emission control of coal combustion and biomass burning. The decreased sulfate contribution and increased nitrate fraction were highly consistent with the much faster emission reductions in sulfur dioxide (SO2) due to phasing out coal in Beijing compared to reduction in nitrogen oxides emissions estimated by bottom-up inventory. The chemical transport model simulations with these emission estimates reproduced the relative changes in aerosol composition and suggested that the reduced emissions in Beijing and its surrounding regions played a dominant role. The variations in meteorological conditions and regional transport contributed much less to the changes in aerosol concentration and its chemical composition during 2014-2017 compared to the decreasing emissions. Finally, we speculated that changes in precursor emissions possibly altered the aerosol formation mechanisms based on ambient observations. The observed explosive growth of sulfate at a relative humidity (RH) greater than 50 % in 2014 was delayed to a higher RH of 70 % in 2017, which was likely caused by the suppressed sulfate formation through heterogeneous reactions due to the decrease in SO2 emissions. Thermodynamic simulations showed that the decreased sulfate and nitrate concentrations have lowered the aerosol water content, particle acidity, and ammonium particle fraction. The results in this study demonstrate the response of aerosol chemistry to the stringent clean air actions and identify that the anthropogenic emission reductions are a major driver, which could help to further guide air pollution control strategies in China.