The Clean Air Status and Trends Network (CASTNet) was established by the U.S. EPA in response to the requirements of the 1990 Clean Air Act Amendments. To satisfy these requirements CASTNet was designed to assess and report on geographic patterns and long-term, temporal trends in ambient air pollution and acid deposition in order to gauge the effectiveness of current and future mandated emission reductions. This paper presents an analysis of the spatial patterns of deposition of sulfur and nitrogen pollutants for the period 1990-2000. Estimates of deposition are provided for two 4-yr periods: 1990-1993 and 1997-2000. These two periods were selected to contrast deposition before and after the large decrease in SO2 emissions that occurred in 1995. Estimates of dry deposition were obtained from measurements at CASTNet sites combined with deposition velocities that were modeled using the multilayer model, a 20-layer model that simulates the various atmospheric processes that contribute to dry deposition. Estimates of wet deposition were obtained from measurements at sites operated bythe National Atmospheric Deposition Program. The estimates of dry and wet deposition were combined to calculate total deposition of atmospheric sulfur (dry SO2, dry and wet SO4(2-)) and nitrogen (dry HNO3, dry and wet NO3-, dry and wet NH4+). An analysis of the deposition estimates showed a significant decline in sulfur deposition and no change in nitrogen deposition. The highest rates of sulfur deposition were observed in the Ohio River Valley and downwind states. This region also observed the largest decline in sulfur deposition. The highest rates of nitrogen deposition were observed in the Midwest from Illinois to southern New York State. Sulfur and nitrogen deposition fluxes were significantly higher in the eastern United States as compared to the western sites. Dry deposition contributed approximately 38% of total sulfur deposition and 30% of total nitrogen deposition in the eastern United States. Percentages are similar for the two 4-yr periods. Wet sulfate and dry SO2 depositions were the largest contributors to sulfur deposition. Wet nitrate, wet ammonium, and dry HNO3 depositions were the largest contributors to nitrogen deposition.
Cloud water deposition was estimated at three high-elevation sites in the Appalachian Mountains of the eastern United States (Whiteface Mountain, NY; Whitetop Mountain, VA; and Clingman's Dome, TN) from 1994 through 1999 as part of the Mountain Acid Deposition Program (MADPro). This paper provides a summary of cloud water chemistry, cloud liquid water content, cloud frequency, estimates of cloud water deposition of sulfur and nitrogen species, and estimates of total deposition of sulfur and nitrogen at these sites. Other cloud studies in the Appalachians and their comparison to MADPro are also summarized. Whiteface Mountain exhibited the lowest mean and median concentrations of sulfur and nitrogen ions in cloud water, while Clingman's Dome exhibited the highest mean and median concentrations. This geographic gradient is partly an effect of the different meteorological conditions experienced at northern versus southern sites in addition to the difference in pollution content of air masses reaching the sites. All sites measured seasonal cloud water deposition rates of SO 4 2Ϫ greater than 50 kg/ha and NO 3 Ϫ rates of greater than 25 kg/ha. These high-elevation sites experienced additional deposition loading of SO 4 2Ϫ and NO 3
Atmospheric concentrations of ammonia (NH3) are not well characterized in the United States due to the sparse number of monitors, the relatively short lifetime of NH3 in the atmosphere, and the difficulty in measuring non-point source emissions such as fertilized agricultural land. In this study, we compare measured weekly concentrations of NH3 collected by two denuder systems with a bi-weekly passive NH3 sampler used by the National Atmospheric Deposition Program's (NADP) Ammonia Monitoring Network (AMoN). The purpose of the study was to verify the passive samplers used by AMoN and characterize any uncertainties introduced when using a bi-weekly versus weekly sampling time period. The study was conducted for 1 year at five remote Clean Air Status and Trends Network (CASTNET) sites. Measured ambient NH3 concentrations ranged from 0.03 μg NH3 m(-3) to 4.64 μg NH3 m(-3) in upstate New York and northwest Texas, respectively, while dry deposition estimates ranged from 0.003 kg N ha(-1) wk(-1) to 0.47 kg N ha(-1) wk(-1). Results showed that the bi-weekly passive samplers performed well compared to annular denuder systems (ADS) deployed at each of the five CASTNET sites, while the MetOne Super SASS Mini-Parallel Plate Denuder System (MPPD) was biased low when compared to the ADS. The mean relative percent difference (MRPD) between the ADS and MPPD and the ADS and AMoN sampler was -38% and -9%, respectively. Precision of the ADS and MPPD was 5% and 13%, respectively, while the precision of the passive samplers was 5%. The results of this study demonstrate that the NH3 concentrations measured by AMoN are comparable to the ADS and may be used to supplement the high-time resolution measurements to gain information on spatial gradients of NH3, long-term trends and seasonal variations in NH3 concentrations.
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