Agricultural ammonia emissions and ammonium concentrations associated with aerosols and precipitation in the southeast United States

[1] Temporal and spatial variations in ammonia (NH3) emissions and ammonium (NH4+) concentrations associated with aerosols and volume-weighted NH4+ concentration in precipitation are investigated over the period 1990-1998 in the southeast United States (Alabama, Florida, Georgia, Kentucky, North Carolina, South Carolina, Mississippi, and Tennessee). These variations were analyzed using an NH3 emissions inventory developed for the southeast United States and ambient NH4+ data from the various Clean Air Status and Trends Network (CASTNet) and the National Atmospheric Deposition Program/National Trends Network (NADP/NTN). Results show that natural log-transformed annual NH4+ concentration associated with aerosols increases with natural log-transformed annual NH3 emission density within the same county (R-2 = 0.86, p < 0.0001, N = 12). Natural log-transformed annual volume-weighted average NH4+ concentration in precipitation shows only a very weak positive correlation with natural log-transformed annual NH3 emission densities within the corresponding county (R-2 = 0.12, p = 0.04, N = 29). Analysis of NH4+ concentration associated with aerosols at CASTNet sites revealed that temperature, precipitation amount, and relative humidity are the most statistically significant (p < 0.05) parameters in predicting the weekly concentrations of NH4+ during the period 1990-1998. Wind speed and wind direction were also statistically significant (p < 0.05) at several CASTNet sites, but the results were less consistent. Investigation into wet NH4+ concentration in precipitation consistently yielded temperature as a statistically significant (p < 0.05) parameter at individual sites. Trends over the period 1990-1998 revealed a slight decrease in NH4+ concentration at CASTNet site SPD, Claiborne County, Tennessee (2.14-1.88 mg m(-3)), while positive trends in NH4+ concentration in precipitation were evident at NADP sites NC35, Sampson County, North Carolina (0.2-0.48 mg L-1) and KY35, Rowan County, Kentucky (0.2-0.35 mg L-1) over the period 1990-1998.