Spatial and Temporal Variations in the Atmospheric Age Distribution of Primary and Secondary Inorganic Aerosols in China

Abstract

The aging timescale of particles is a key parameter in determining their impacts on air quality, human health, and climate. In this study, a one-year simulation of the age distributions of the primary and secondary inorganic fine particulate matter (PM2.5) components was conducted over China using an age-resolved Community Multiscale Air Quality (CMAQ) model. The results indicate that primary PM2.5 (PPM) and ammonium mainly originate from fresh local emissions, with approximately 60%–80% concentrated in 0–24 h age bins in most of China throughout the year. The average age is about 15–25 h in most regions in summer, but increases to 40–50 h in southern region of China and the Sichuan Basin (SCB) in winter. Sulfate is more aged than PPM, indicating an enhanced contribution from regional transport. Aged sulfate with atmospheric age > 48 h account for 30%–50% of total sulfate in most regions and seasons, and the concentrations in the > 96 h age bin can reach up to 15 µg·m−3 in SCB during winter. Dramatic seasonal variations occur in the Yangtze River Delta, Pearl River Delta, and SCB, with highest average age of 60–70 h in winter and lowest of 40–45 h in summer. The average age of nitrate is 20–30 h in summer and increases to 40–50 h in winter. The enhanced deposition rate of nitric acid vapor combined with the faster chemical reaction rate of nitrogen oxides leads to a lower atmospheric age in summer. Additionally, on pollution days, the contributions of old age bins (> 24 h) increase notably for both PPM and secondary inorganic aerosols in most cities and seasons, suggesting that regional transport plays a vital role during haze events. The age information of PM2.5, provided by the age-resolved CMAQ model, can help policymakers design effective emergent emission control measures to eliminate severe haze episodes.