Historical gaseous and primary aerosol emissions in the United States from 1990 to 2010

An accurate description of emissions is crucial for model simulations to reproduce and interpret observed phenomena over extended time periods. In this study, we used an approach based on activity data to develop a consistent series of spatially resolved emissions in the United States from 1990 to 2010. The state-level anthropogenic emissions of SO2, NOx, CO, NMVOC (non-methane volatile organic compounds), NH3, PM10 and PM2.5 for a total of 49 sectors were estimated based on several long-term databases containing information about activities and emission controls. Activity data for energy-related stationary sources were derived from the State Energy Data System. Corresponding emission factors reflecting implemented emission controls were calculated back from the National Emissions Inventory (NEI) for seven years (i.e., 1990, 1995, 1996, 1999, 2001, 2002 and 2005), and constrained by the AP-42 (US EPA's Compilation of Air Pollutant Emissions Factors) dataset. Activity data for mobile sources including different types of highway vehicles and non-highway equipment were obtained from highway statistics reported by the Federal Highway Administration. The trends in emission factors for highway mobile source were informed by the 2011 National Transportation Statistics. Emissions for all non-energy-related sources were either scaled by the growth ratio of activity indicators or adjusted based on the NEI trends report. Because of the strengthened control efforts, particularly for the power sector and mobile sources, emissions of all pollutants except NH3 were reduced by half over the last two decades. The emission trends developed in this study are comparable with the NEI trend report and EDGAR (Emissions Database for Global Atmospheric Research) data, but better constrained by trends in activity data. Reductions in SO2, NOx, CO and EC (speciation of PM2.5 by SMOKE, Sparse Matrix Operator Kernel Emissions) emissions agree well with the observed changes in ambient SO2, NO2, CO and EC concentrations, suggesting that the various controls on emissions implemented over the last two decades are well represented in the emission inventories developed in this study. These inventories were processed by SMOKE and are now ready to be used for regional chemistry transport model simulations over the 1990-2010 period.