1Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Canada
2NOAA Earth System Research Laboratory, Boulder, CO, USA
3Environment Canada, Downsview, Toronto, Canada
4Electric Power Research Institute, Palo Alto, CA, USA
Abstract. Nucleation in coal-fired power-plant plumes can greatly contribute to particle number concentrations near source regions. The changing emissions rates of SO2 and NOx due to pollution-control technologies over recent decades may have had a significant effect on aerosol formation and growth in the plumes, with ultimate implications for climate and human health. We use the System for Atmospheric Modeling (SAM) large-eddy simulation model with the TwO-Moment Aerosol Sectional (TOMAS) microphysics algorithm to model the nucleation in plumes of coal-fired plants. We test a range of cases with varying emissions to simulate the implementation of emissions-control technologies between 1997 and 2010. For the W.A. Parish power plant (near Houston, TX) during this time period, NOx emissions were reduced by ~90%, while SO2 emissions decreased by ~30%. Increases in plume OH (due to the reduced NOx) produced enhanced SO2 oxidation and particle nucleation despite the reduction in SO2 emissions. These results suggest that NOx emissions may strongly regulate particle nucleation and growth in power-plant plumes. Comparison of model results with airborne measurements made in the W.A. Parish power-plant plume in 2000 and 2006 confirm the importance of NOx emissions on new particle formation, yet also highlight the substantial effect of background aerosol loadings on this process. A wide range of NOx and SO2 emissions were modeled to understand how they affect particle formation in the plume. Particle formation generally increases with SO2 emission, while NOx shows two different regimes: increasing particle formation with increasing NOx under low-NOx emissions and decreasing particle formation with increasing NOx under high-NOx emissions. Finally, we calculate emissions statistics of 330 coal-fired power plants in the US in 1997 and 2010, and the model results show a median decrease of 19% in particle formation ratesfrom 1997 to 2010 (whereas the W.A. Parish case study showed an increase). These results suggest that there may be important climate implications of power-plant controls due to changes in plume chemistry and microphysics. More extensive plume measurements for a range of emissions of SO2 and NOx and in varying background aerosol conditions are needed to better quantify these effects.