Simulation of airborne trace metals in fine particulate matter over North America

Trace metal distributions are of relevance to understand sources of fine particulate matter (PM_2.5), PM_2.5-related health effects, and atmospheric chemistry. However, knowledge of trace metal distributions is lacking due to limited ground-based measurements and model simulations. This study develops a simulation of 12 trace metal concentrations (Si, Ca, Al, Fe, Ti, Mn, K, Mg, As, Cd, Ni and Pb) over continental North America for 2013 using the GEOS-Chem chemical transport model. Evaluation of modeled trace metal concentrations with observations indicates a spatial consistency within a factor of 2, an improvement over previous studies that were within a factor of 3-6. The spatial distribution of trace metal concentrations reflects their primary emission sources. Crustal element (Si, Ca, Al, Fe, Ti, Mn, K) concentrations are enhanced over the central US from anthropogenic fugitive dust and over the southwestern U.S. due to natural mineral dust. Heavy metal (As, Cd, Ni and Pb) concentrations are high over the eastern U.S. from industry. K is abundance in the southeast from biomass burning and high concentrations of Mg is observed along the coast from sea spray. The spatial pattern of PM_2.5 mass is most strongly correlated with Pb, Ni, As and K due to their signature emission sources. Challenges remain in accurately simulating observed trace metal concentrations. Halving anthropogenic fugitive dust emissions in the 2011 National Air Toxic Assessment (NATA) inventory and doubling natural dust emissions in the default GEOS-Chem simulation was necessary to reduce biases in crustal element concentrations. A fivefold increase of anthropogenic emissions of As and Pb was necessary in the NATA inventory to reduce the national-scale bias versus observations by more than 80 %, potentially reflecting missing sources.