Atmospheric Age Distribution of Primary and Secondary Inorganic Aerosols in a Polluted Atmosphere.

The community multiscale air quality (CMAQ) model was modified to track the evolution of the atmospheric age (τ) distribution of primary particulate matter (PPM) and secondary inorganic aerosol components (nitrate, sulfate, and ammonium ion, NSA). The modified CMAQ gas and aerosol mechanisms represent the same species emitted at different times as an age-resolved mixture, using multiple age-tagged variables and a dynamic age-bin advancing scheme. The model was applied to study the spatial and temporal evolution of τ for PPM and NSA in January 2013 to understand the formation and regional transport of PM and the precursor gases during severe winter pollution episodes in China. The results showed that increases in PPM and NSA concentrations during high pollution periods in polluted urban areas were typically associated with increases in the mean atmospheric age (τ̅) due to the accumulation of local emissions and regional transport of aged pollutants. Some of the rapid sulfate growth events at the beginning of multiday air pollution episodes were driven by regional transport of aged particles. In heavily polluted cities, while most of the monthly average PPM had τ less than 10 h, more than half of the sulfate had τ greater than 20-30 h. Regional distributions showed that very aged sulfate particles with τ > 96 h accounted for a significant portion of the total sulfate and had a very broad spatial distribution. However, aged ammonium ions had very low concentrations. Aged nitrate also had lower concentrations and more limited spatial distributions than sulfate due to differences in the atmospheric lifetime between SO2 and NOx. The estimated NOx lifetime of approximately ∼24 h in China agrees with a satellite-based estimation of 21 h. Potential applications of the age distribution analysis include evaluating the impacts of meteorology on air quality and developing short-term emission control strategies.