Effects of changes in sulfate, ammonia, and nitric acid on particulate nitrate concentrations in the southeastern United States.

A thermodynamic equilibrium model, Simulating Composition of Atmospheric Particles at Equilibrium (SCAPE2), was used to investigate the response of fine particulate NO3(-) to changes in concentrations of HNO3, NH3, and SO4(2-) in the southeastern United States. The data consisted of daily, 24-hr time resolution measurements from the Aerosol Research Inhalation Epidemiology Study (ARIES) Jefferson Street (Atlanta) site and five other sites of the Southeastern Aerosol Research and Characterization Project (SEARCH). Reductions of total NH3 (gas-phase NH3 plus particulate NH4(+)), total NO3(-) (HNO3 plus particulate NO3(-)), SO4(2-), or combined total NO3(-) (HNO3 plus particulate NO3(-)) with SO4(2-) were used to estimate the effects of changing emission levels. The conversion of SO2 to SO4(2-) and NO2 to HNO3 involves additional nonlinear reactions not incorporated into the model. For all sites, fine particulate NO3(-) concentrations decreased in response to reductions of either NH3 or total NO3(-), but the particulate NO3(-) decreases were greater for the NH3 reductions than for the total NO3(-) reductions. Particulate NO3(-) concentrations increased in response to reductions of SO4(2-). For the combined reduction (total NO3(-) plus SO4(2-)), the resulting particulate NO3(-) concentrations were on average no different than the base-case NO3(-) levels. Measurements of fine particulate NO3(-) and HNO3 support the modeling conclusions and indicate that particulate NO3(-) formation is limited by the availability of NH3 at most times at all SEARCH sites.